Production I.G's anime series Psycho-Pass features characters designed by manga artist Akira Amano. The anime takes place in a dystopia where citizens are continuously assessed via omnipresent cymatic scans used to determine their mental state, personality, and the probability that they will commit crimes. The result of said reading is labeled one's Psycho-Pass.

Throughout its three seasons, viewers follow the members of Unit One (aka Division One) of the Ministry of Welfare Public Safety Bureau's Criminal Investigation Division supported by the Sibyl System.

Director Naoyoshi Shiotani decided on how to make the series' characters after hearing comments from The Pet Girl of Sakurasou's director Atsuko Ishizuka. As that for that series the characters were designed first, Shiotani realized it was the opposite for them. They had to create the setting first and then continue with the characters as they "are almost being played by the world." As a result, the cast was designed by manga artist Akira Amano in order to make them balance with the dark atmosphere by having them "palatable and very relate-able." The staff also avoided using bright colors that would stand out. These designs were adapted by character designer Kyoji Asano.

Akane Tsunemori was created as the most relatable character who would question the setting from the audience's point of view and as the heroine who would come between Shinya Kogami and Shogo Makishima. Her growth in the series from an innocent rookie to a mature and haunted person was one of the staff's main objectives. Whenever an episode included violent scenes where the main characters were involved, the team worked on them to make them memorable. As the series was "anti-moe" the team decided to avoid having Akane remove her clothes and instead have Kogami do it. The staff also decided to focus more on friendships rather than romantic relationships. Voice actors have also been credited in the making of the series due to how they added traits to the characters.

Season One is seen through the eyes of Akane Tsunemori, a rookie Inspector in charge of solving cases with veteran Inspector Nobuchika Ginoza and their team of Enforcers, most notably Shinya Kogami, a former Inspector seeking vengeance on criminal Shogo Makishima. Tsunemori returns in Season Two as the leader of Unit One, with a re-organized team hunting down criminal Kirito Kamui. Psycho-Pass: The Movie has Tsunemori leaving Japan in order to bring her team to Shambala Float where she runs into her former ally, Kogami, now an expatriate become resistance fighter. The trilogy Sinners of the System tells independent stories that focus on some characters while the Season Three series introduces a new Unit One with Arata Shindo and Kei Mikhail Ignatov as rookie Inspectors who uncover a shadowy organization known as Bifrost.

Akane Tsunemori is the 20-year-old main heroine - point-of-view character and the newly assigned Inspector of Unit One. She passes the exams with the highest score for employment on several public sectors and private corporations. She decides to join the police because it is the only place where no one obtained a score as high as hers, thus she believes she is able to do something there that no one else can. Though initially uncomfortable with her job, Kogami's joy of having somebody who would stop him from killing innocent people motivates her to work and get along with the Enforcers. Her calm demeanor, acceptance of society and will to fight to against conflicts prevent her from becoming a latent criminal despite her experiences. The members from the Sibyl System are attracted by her traits which results in her learning of their true nature as they want to use her to capture Makishima alive with Akane agreeing only if they stop their orders of killing the defecting Kogami. Although she fails, the Sibyl members allow her to live under the condition she does not reveal their truth. In the epilogue, Akane becomes the de facto leader of Unit One. Akane is seen briefing a newly recruited Inspector in the finale. She continues leveraging her position as a trusted Inspector with a personal connection to the Sibyl System until she is arrested before the start of Season 3, forcibly demoting her. She is voiced by Kana Hanazawa in Japanese and by Kate Oxley in English.

Shinya Kōgami is the 28-year-old main protagonist and Enforcer in Unit One. Formerly an Inspector, his involvement in the Specimen Case caused his Crime Coefficient to rapidly increase to abnormal levels. While investigating the case, Mitsuru Sasayama, the Enforcer that worked under him, was on to the mastermind behind the case until he was killed in the same manner as the victims. Instead of seeking the needed therapy, Shinya became so focused on the case that he was demoted to Enforcer by the Sibyl System, restricting his freedom and limiting his movement to inside the Public Safety Bureau. Despite his violent actions, Kogami feels relaxed when Akane Tsunemori is assigned as his Inspector as he believes he will be a detective rather than a killer under her judgement. As an Enforcer, Kogami takes extensive physical training so that his superiors will not have to kill criminals. The two manage to arrest Makishima but following his escape, Kogami is taken off the case due to the Sibyl not wishing Makishima dead. As a result, Kogami leaves Unit One to hunt down and kill Makishima alone. He ultimately succeeds and is not seen again by his comrades, although in the audio drama After Stories he contacts Akane about how he will stay away from society in order to avoid being detected. He is voiced in Japanese by Tomokazu Seki and in English by Robert McCollum.

Nobuchika Ginoza is a veteran Inspector working with Akane. He coordinates all the Enforcers in Unit One. An old friend of Shinya's, his hatred for those with high Crime Coefficients and his zeal to oust them from society came from the inability to stop his former partner from becoming a latent criminal. Although he still holds a certain degree of trust with Shinya, he dislikes Shinya's Enforcer partner Masaoka, his father. His father's demotion to Enforcer causes Ginoza to constantly tell Akane to draw a line between herself and the Enforcers she works with. During the group's search for Makishima, Masaoka sacrifices his life to save his son from Makishima's dynamite and Ginoza loses an arm shortly afterwards. Ginoza's Crime Coefficient rises too high and he is demoted to an Enforcer, mirroring the fates of his father and Kogami. Despite this, Gen Urobuchi wrote Ginoza Nobuchika as a more sympathetic toward both Akane and Kogami for the 2015 movie where he assists the missing Kogami in a fight. In regards to the first Sinners of the System film, Shiotani picked Nobuchika Ginoza and Mika Shimotsuki as the main characters due to their similarities to the protagonists from the first television series, Shinya Kogami and Akane Tsunemori, respectively. Nevertheless, he noted this duo employed a different dynamic from Kogami and Akane while noting how Ginoza has undergone a notable character arc across the previous projects related to Psycho-Pass mainly due to his relationship with Masaoka and Kogami. He is voiced by Kenji Nojima in Japanese and Jessie James Grelle in English.