- Misaki Suzuhara (鈴原 みさき Suzuhara Misaki?)
- Misaki is a very timid, sweet-tempered, and kind (although shown in the manga to be more overreactive and easily excited) 12-year-old girl who has just moved to Tokyo to live with her aunt. She had been living with her grandparents in Wakayama while she went to elementary school, but saved up money that her mother had been sending her while she was away so she could afford to go to middle school in Tokyo. She also worries about the fact that she is small and unathletic, and is sometimes mistaken to be in elementary school, but sees Angelic Layer as a way to prove to others and herself that there is nothing wrong with being small. She started playing Angelic Layer after seeing the white angel Athena on a video screen outside of Tokyo Station (unaware that she was seeing her own mother's Angel). Her angel is Hikaru and she is known as the "Miracle Rookie". She is nicknamed Misakichi (みさきち) by her friend Tamayo to make her name sound cute.
- Ichiro Mihara (三原 一郎 Mihara Ichirō?)
- Nicknames himself Icchan (いっちゃん) to hide his true identity from Misaki. He is 28 years old and oftens acts extremely eccentric, spontaneous and immature for his age. (often jumping out of random places shouting "Icchan go BOOM!" to scare Misaki and Ogata), but nonetheless is ingenious and dead serious when it comes to Angelic Layer. In the manga, Icchan is the president of the Piffle Company that creates the Angelic Layer toys. In the anime, Icchan is the "father" of Angelic Layer and creator, having developed the game over seven years with the help of Shuko Suzuhara. Icchan had been an employee at a hospital trying to treat Shuko's neurological condition and were developing the angels as part of research to create prosthetic limbs which could be controlled by brain waves. However, research funds were cut off after the hospital thought that the research was costing too much. As a result, Icchan and Shuko created Angelic Layer in order to help fund and conduct further research.
- Crossover: Icchan is the late husband of Chitose Hibiya and the creator of the persocoms in the hit manga Chobits. He made two special persocoms, the Chobits, for his wife to be their children, since she could not have children herself. They were named Freya and Elda, later known as Chi. The Chobits were created from the findings gathered from the research performed for Angelic Layer project. The cause of his death in Chobits is that he died of an illness.
Hatoko Kobayashi (小林 鳩子 Kobayashi Hatoko?)
- Angel Entry Phrase: "Exceed the speed of light and sound, Suzuka!"
- Date of birth: December 07, 1991
- Voiced by: Yuri Shiratori (Japanese), Sasha Paysinger (English)
- Hatoko is a 5 year old known as the "Miracle Kindergartner" and is Misaki's best friend and Angelic Layer mentor. Even at a very young age, she is extremely intelligent, mature, and hard-working. She is an expert at Angelic Layer, often winning her games in mere seconds. She wins all ten of her games at the Tokyo prefecture games, and is the defending champion of the Kantō regional games. She is fiercely competitive, working to increase her angel's speed and power often. She also likes to poke fun at her brother Kotaro for his apparent ineptness when it comes to his crush on Misaki. Hatoko also treats Misaki like her student rather than her nee-chan (sister) and is also her mentor. Hatoko's angel is Suzuka.
Kotaro Kobayashi (小林 虎太郎 Kobayashi Kōtarō?)
- Date of birth: September 04, 1984
- Voiced by: Jun Fukuyama (Japanese), Kevin Corn (English)
- Kotaro is a 13 year old middle school classmate of Misaki, whom he has a crush on, as well known as Hatoko's brother. He is always being assaulted by Tamayo and her various martial arts techniques, which he has been a victim of since he was four years old. He becomes jealous of Ohjiro's advances towards Misaki, going so far as to try to attempt to play a quasi-match of Angelic Layer against Ohjiro, despite the fact that he had never played it before. His family owns a karate dojo and Kotaro has practiced karate some himself, showing Misaki some of his knowledge in hopes that Misaki can use it to help Hikaru win. In the manga, he and Misaki later fall in love and date. He also resembles Hiromu Shinbo from Chobits.
Tamayo Kizaki (木崎 珠代 Kizaki Tamayo?)
- Date of birth: April 17, 1984
- Voiced by: Satsuki Yukino (Japanese), Monica Rial (English)
- Tamayo is 13 years old and is a friend and classmate of Misaki. She nicknames Misaki "Misakichi" and is rather eccentric. One of her favorite activities is practicing her martial arts techniques on her unwilling friend Kotaro. She always loudly cheers for Misaki at Angelic Layer matches and defends her against those who question her ability. In the anime, it is later revealed that Tamayo has always held intimate feelings for Kotaro, while in the manga, she only saw him as a close friend. She offers to be Misaki's "second" in her national game match against the Angelic Layer Company's angel due to Hatoko becoming ill before Misaki accepts Ohjiro's offer to be her second.
- The various martial arts Tamayo has mastered after eight years of hard training are: wrestling, karate, K-1, kenpō, boxing, judo, capoeira, and taekwondo.
- In the anime she finally ends up with Kotaro after finally telling him how she feels (despite the fact Kotaro initially liked Misaki). However, in the manga, Tamayo falls in love with Ohjiro Mihara.
Ohjiro Mihara (三原 王二郎 Mihara Ōjirō?)
- Angel Entry Phrase: Unknown
- Date of birth: October 20, 1982
- Voiced by: Soichiro Hoshi (Japanese), Chris Patton (English)
- Ohjiro is 17 years old. He's Icchan's younger step-brother. He has been involved with Angelic Layer for many years, in a large part because it was what brought him and Icchan together after their parents married each other. Ohjiro competes in Kobe and has been the champion of the Kansai Regional games, as well as being the runner-up in the national tournament for two consecutive years. He has a desperate desire to defeat Shuko Suzuhara's angel Athena to get over a childhood crush he had on her. His angel is Wizard. In the anime it is revealed that he is falling in love with Misaki, but he develops a love for both Shuko and Misaki. In the manga, he has no feelings for Misaki or Shuko, but likes Tamayo.
Shuko Suzuhara (鈴原 萩子 Suzuhara Shūko?)
- Angel Entry Phrase: "Athena's wings! Open up the future!"
- Date of birth: November 28, 1965
- Voiced by: Kikuko Inoue (Japanese), Christine M. Auten (English)
- Shuko is Misaki's mother and Shoko's elder sister. She is 31 years old. In the anime, it is explained that Shuko left a 5-year-old Misaki to be taken care of her grandparents under the guise of work, when in reality she was going to Tokyo in order to find a way to cure the neurological disease she had been inflicted with. This disease inhibits nerve signals from reaching to or from her legs. Ichiro Mihara was a doctor attempting to work with her to find a cure when the two started Angelic Layer as a way to do research and raise funds when their original research funding was cut off. Shuko, or "Shu" as she is called when playing Angelic Layer, is the undisputed champion with her angel Athena, having won each of the past three national championships. Over the past seven years, she has avoided meeting Misaki, afraid of what Misaki would think of her. In the manga, however, Shuko has no such disease and is merely extremely shy about socializing with those she loves. She also works for the company behind Angelic Layer.
Sai Jounouchi (城乃内 最 Jōnouchi Sai?)
- Angel Entry Phrase: Let the silver snow fall! Dance, Shirahime!
- Date of birth: February 15, 1980
- Voiced by: Houko Kuwashima (Japanese), Tiffany Grant (English)
- 16 year old Sai Jounouchi, known as the "Ice Machine," started playing Angelic Layer at the request of her terminally ill sister Rin. Rin designed what the angel would look like, but died before Sai could create her. As a result, Sai states that her reason for playing Angelic Layer is "to become strong." Sai is from Kanagawa Prefecture and was the runner-up in the Kantō Regional games in the past year. She is friends with Kaede, who went to the same middle school as Sai. Her angel is Shirahime.
Kaede Saito (斉藤 楓 Saitō Kaede?)
- Angel Entry Phrase: Blanche! Everything is at your will!
- Date of birth: October 14, 1981
- Voiced by: Ayako Kawasumi (Japanese), Tiffany Terrell (English)
- Kaede is a 15 year old quiet and wise girl from Kanagawa and is friends with Sai Jounouchi. Her parents divorced and she lives with her father. She received an angel egg as a gift from someone in her father's company. Her personality does not appear to be one suited for Angelic Layer, as pointed out by her father when he comments that he never believed that he would see Kaede compete in a fighting game. Despite this, she is very adept at Angelic Layer. She treats her angel, Brunashe, as her own daughter.
- She also appears in Chobits as Minoru Kokubunji's late older sister.
Masaharu Ogata (尾形 雅治 Ogata Masaharu?)
- Date of birth: August 27, 1973
- Voiced by: Tomokazu Seki (Japanese), Mark Laskowski (English)
- Ogata(age 24) is one of Icchan's subordinates in the Angelic Layer control room and lab. Icchan often ensnares Ogata into situations that result in Ogata getting "penalized." These penalties involve a range of embarrassing or terrible things, such as having a live octopus being stuck down his pants or being made to eat spaghetti through his nose. Icchan also named a remarkably ugly angel after him as a penalty.
Shoko Asami (浅見 祥子 Asami Shōko?)
- Date of birth: August 12, 1971
- Voiced by: Kotono Mitsuishi (Japanese), Kelly Manison (English)
- Shoko is Misaki's aunt and Shuko's younger sister. She's 26 years old. She demands that Misaki and her friends call her "Miss Shoko" instead of "aunt" ("obasan" in Japanese) because she is still "an attractive young newscaster." She often covers Angelic Layer events for the local news station that she works for. Misaki lives with Shoko when she moves to Tokyo.
- Her hairstyle bears a resemblance to that of Takako Shimizu in Chobits.
Ringo Seto (瀬戸 林子 Seto Ringo?)
- Angel Entry Phrase: Start dancing, Ranga!
- Date of birth: May 24, 1983
- Voiced by: Kana Ueda (Japanese), Mariela Ortiz (English)
- Ringo is a 14 year old pop idol from Tochigi who plays Angelic Layer over the objections of her manager. In order to become strong and beat Hikaru, she studies Hikaru's past battles, notably against Suzuka because she didn't lose quickly. Ringo likes living freely and often escapes from her manager to get out of doing work. When Misaki was fighting her male classmate Ryo Misaki in a set of Angelic Layer matches, Ringo encouraged Misaki on between matches. Ringo's angel is Ranga.
Madoka Fujisaki (藤崎 円香 Fujisaki Madoka?)¹
- Angel Entry Phrase: Hit! Slash! Break! Mao's fist is my fist! The Angel descends!
- Date of birth: October 27, 1984
- Voiced by: Tomoko Kawakami (Japanese), Shelley Calene-Black (English)¹
- Madoka is a strong competitor in the Kantō Regional games who fights against Suzuka and Hikaru, losing to both. Madoka is a Kung Fu artist, using martial arts as her angel's chief fighting tactics. She has a strong desire to defeat Hatoko Kobayashi's angel, Suzuka to recover her family's "lost pride". While spectating Hikaru's fight against another contestant, she and her sister make it clear to Kaede Saito and Sai Jonouchi that she will not lose to anyone until after Suzuka is defeated. Arisu and Madoka sabotage Hikaru with a transmitter that will block Misaki's thoughts from reaching her doll in the hopes of winning, but are caught by Ohjiro Mihara. After losing, Madoka obtains a new outlook on why people play Angelic Layer and realizes that it was made to be fun for any person, to the slight annoyance of her sister. Madoka's angels are created by her younger sister, Arisu.
Arisu Fujisaki (藤崎 有栖 Fujisaki Arisu?)²
- Angel Entry Phrase: Unknown
- Date of birth: June 25, 1987
- Voiced by: Chiemi Chiba (Japanese), Mandy Clark (English)²
- Arisu is a talented genius Angel-builder who aids her sister in creating Angels. She follows in her sister's steps as a talented Kung Fu artist, and creates very strong and agile angels. Arisu does not make Angels for herself, suggesting that she is not good at guiding them. Arisu designed Mao and Unpyo to be stronger than Suzuka, but Unpyo loses to Suzuka in record time, which mortifies her and her sister. After sabotaging Hikaru with a transmitter, Arisu is caught by Ohjiro Mihara and is told that Angelic Layer is meant to show true talent and that anyone can be brilliant, thus forcing her to give up cheating to win. She is very sensitive about the Angels she builds, and accuses her sister of not liking the Angels she made after their loss to Hikaru. Arisu creates a balance oriented Angel for herself near the end of the anime, called Arisu, and vows to beat Hikaru in a friendly battle. At the end credits, in the last episode, Arisu is shown fighting the angel Queen with Alice.
- Arisu's name is translated in the Japanese anime credits as "Alice".
Hiromi Fujimori (藤森 ひろみ Fujimori Hiromi?)
- Voiced by: Yui Horie (Japanese), Allison L. Sumrall (English)
Yuko Inada (稲田 夕子 Inada Yūko?)
- Voiced by: Hiromi Nishikawa (Japanese), Kaytha Coker (English)
Shuji Inada (稲田 修二 Inada Shūji?)
- Voiced by: Yoshiyuki Kono (Japanese), Jay Hickman (English)
Angelic Layer Host (司会者 Shikaisha?)
- Voiced by: Yoshiyuki Kono (Japanese), Vic Mignogna (English)
Kyoko (京子 Kyōko?)
- Voiced by: Chieko Atarashi (Japanese), Luci Christian (English)
Asuka Kitamura (北村 飛鳥 Kitamura Asuka?)
- Voiced by: Mamiko Noto
Yuko Hikawa (氷川 優子 Hikawa Yūko?)
- Voiced by: Sayaka Ohara
Tomoko Yamada (山田 知子 Yamada Tomoko?)
- Voiced by: Mayumi Asano (Japanese), Kaytha Coker (English)
Maria Shibata (柴田 まりあ Shibata Maria?)
- Voiced by: Kazusa Murai (Japanese), Hilary Haag (English)
Ryo Misaki (岬 了 Misaki Ryō?)
- Voiced by: Kappei Yamaguchi (Japanese), Kira Vincent-Davis (English)
Rin Jounouchi (城乃内 鈴 Jōnouchi Rin?)
- Voiced by: Sayuri Yoshida (Japanese), Allison Sumrall (English)
Chitose Tanaka (田中 千歳 Tanaka Chitose?)
- Voiced by: Tomoko Miura (Japanese), Kim Prause (English)
Tsubasa "The Blonde Gale" McEnzie (つばさ・マッケンジー Tsubasa Makkenjī?)
- Voiced by: Rio Natsuki (Japanese), Shelley Calene-Black (English)
Hikaru (ヒカル Hikaru?) - Deus: Misaki Suzuhara
- Though small and lightweight compared to most Angels, Hikaru possesses very strong attacks, most which are speed based. Her small stature makes her aerodynamically quick and agile. She was created by Misaki in order to show others that there was nothing wrong with being small through Angelic Layer. Her basic appearance is a bit tomboyish, since Misaki had accidentally cut her hair short, and has a less mature physique than other Angels. Hikaru also appears as a crossover character in Chapter 144 of Clamp's manga Tsubasa: Reservoir Chronicle. Hikaru's name can also mean 'glowing' or 'shining' in Japanese. In the manga, Misaki bases Hikaru's appearance on a character from a manga she read which is Rayearth.
Suzuka - Deus: Hatoko Kobayashi
- Nicknamed “The Speed of Light,” Suzuka often defeats her opponents with incredible speed. For an Angel that was created by 5-year-old Hatoko, Suzuka resembles a beautiful and extremely strong ninja, and her 'Rolling Thunder' attack can defeat other Angels within seconds. Her strength has led her to compete in the heated National Tournament along with Hikaru. Suzuka's name possibly derives from the fact that she adorns two suzus on her bow, and one hanging from her hair.
Shirahime (白姫 Shirahime?, lit. "White Princess") - Deus: Sai Jounouchi
- Nicknamed “The White Princess,” Shirahime is a heavyweight Angel which wears a white kimono. Shirahime's style of fighting is graceful and powerful, and she defeats her opponents with great beauty and strength. Shirahime has finished 2nd in the Kantō regional games for two consecutive years. She fights against Suzuka, and defeats her, and against Athena and Hikaru, losing. She is also capable of reaching "Hypermode" like Blanche.
Blanche (ブランシェ Buranshe?) - Deus: Kaede Saitou
- Nicknamed "The White Angel," Blanche is a powerful angel dressed as a nurse which is so fast that she has only been touched by four other angels. When in a very tough fight, Blanche will use a technique called "Hypermode" which is a result of a glitch present in the first angels built. Blanche is a contestant in the Kantō regional games. Her name can also be written Branche with the romaji "r" sounding like an "l". Blanche is French for white.
Ranga (ランガ Ranga?) - Deus: Ringo Seto
- Ranga uses a technique called "the Dance of Death" which uses wind to attack her opponents from a distance. Ranga is a contestant in the Kantō regional games. She wears Arabic clothes and even resembles Tatra from Magic Knight Rayearth and Sumomo from Chobits. In the end of the anime Ringo is wearing a cosplay of Ranga. In the manga, her name is Lanka, due to different translation.
Wizard (ウィザード Wizādo?) - Deus: Ohjiro Mihara
- Wizard is the Kansai Regional champion and has finished as the runner up in the National Games for two consecutive years. Wizard uses a technique called “Magic Guard” to block his opponent’s attacks with an electric shield that uses static electricity. Misaki was able to neutralize its shield by using one of Hikaru's cables as an earth contact to the layer. Wizard is one of the few male angels in the Layer. He has some resemblance to Clef, from Magic Knight Rayearth.
Athena (アテナ Atena?) - Deus: Shuko Suzuhara
- Athena has won the National Games championship in all three years of its existence and is the undisputed champion of Angelic Layer. It can create powerful powerballs, called Astral Emission, and fly with wings. During their fight Hikaru also learned to do this.
Mao (猫 Mao?) - Deus: Madoka Fujisaki
- The newest angel created by Madoka's sister Arisu. Mao is a contestant in the Kantō regional games. She is designed after a cat, complete with ears and a tail. Mao is Chinese for "cat".
Shadow Panther - Deus: unknown
- The first angel that Hikaru fights and defeats.
Queen - Deus: Kyoko
- An angel which uses electric whips, which are illegal, in unofficial games to easily defeat inexperienced players. She fights and loses to Hikaru in her second Angelic Layer match. In the last episode during the credits, Queen is seen fighting Arisu Fujisaki's angel Alice.
Colossus - Deus: Asuka Kitamura
- An angel which participates in the Tokyo Prefecture games, losing to Hikaru.
Nightingale - Deus: unknown
- An Angel with experience in the Kantō regional games and who is competing in the Tokyo prefecture games. She is defeated by Suzuka in 5 seconds. Nightingale is also defeated by Hikaru in the Tokyo prefecture games.
Katalina - Deus: Yuko Hikawa
- Katalina fights by “skating” on the layer, and uses her skates to attack while spinning. She loses to Hikaru in the first round of the Tokyo prefecture games.
Vasquez - Deus: Tomoko Yamada
- A very powerful angel which lures her opponents into surprise attacks. She is defeated by Hikaru in the second round of the Tokyo prefecture games.
Tsubaki - Deus: Maria Shibata
- An angel defeated by Hikaru in the final round of the Tokyo prefecture games.
Ace, Mark II, & Tri - Deus: Ryo Misaki
- Ryo uses these three angels in a best of three match against Misaki in an attempt to show that girls cannot beat boys at Angelic Layer.
Misaki-chi - Deus: Ryo Misaki
- Ryo made this angel after his lose to Misaki and Hikaru.
Natasha - Deus: unknown
- Champion of the Chiba prefecture games. She is defeated by Suzuka in the first round of the Kantō regional games.
Yusari - Deus: unknown
- An angel competing in the Kantō regional games, losing to Blanche there.
Eagle - Deus: Tsubasa "The Blond Gale" McEnzie
- An angel who competed in the Kyūshū Regional games, she competes against Shirahime in the Angelic Layer National Games. She has the ability to glide through the air using wings, and uses this tactic against Shirahime, although apparently it was not seen during the Kyūshū regionals.
Elain - Deus: Chitose Tanaka
- The "Northern Aurora" an angel from Hokkaidō, she fights Hikaru in the first round of the Angelic Layer National Games. She uses a technique called the "Hexagon Reversion" to immobilize her opponents in mid-air. Along with the lightning storm during Hikaru and Elain's fight, this technique almost make the layer disappear. Elain has obvious advantage on the layer due to the fact that she is a larger angel with long arms.
New Type SI-174 - Deus: Shuji Inada
- An angel competing in the National Games representing the Angelic Layer company. SI-174 is a new model of angel which is capable of quicker and more efficient movements. The SI-174 fights Hikaru in the second round of the National Games.
Alice - Deus: Arisu Fujisaki
- An angel developed by Arisu for herself, in contrast to those she had made for her sister. Her Deus, after seeing Mao lose to Hikaru, competed in other district competitions, and ended up as a finalist for the National Games as an opponent to Hikaru. Alice is a balance-oriented angel, allowing it to stay upright on an icy layer.