The Millennium Earl is the story’s main antagonist. He is a sorcerer from long ago, and he plans to lead the world to its death. He tricks people who mourn for their dead relatives and friends into resurrecting them, turning them into akuma that he can then control. The Earl resembles a grotesque caricature of a Victorian gentleman, a rotund figure in cape and top hat, with a perpetual enormous grin and pince-nez spectacles. Despite his intentions, he often displays a cheerful attitude. He also is shown to have a human form although his facial features are not shown, as mentioned by another character. He is able to control Noah’s Ark and has created a new one, intending to discard the old one when it falls into the possession of the Black Order. He is voiced by Junpei Takiguchi in Japanese and Jason Liebrecht in English.

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Lavi is a cheerful 18 year old, red-haired Exorcist of mixed race. He aims to become a Bookman, a person who records the hidden history of the world and has been trained from a young age to achieve that goal. Lavi is the 49th alias he assumed after casting away his real name to reach it. He works along the Black Order just to be close to the events that must be seen and slowly becomes more attached to his Black Order friends and his original Bookman self is constantly being clouded by his growing care. His anti-akuma weapon, simply named Tettsui and referred to as Ōzuchi Kozuchi is capable of growing and extending to undefined sizes and lengths. Although this affects its weight, it does not affect Lavi. The weapon allows him to use "seals" that control several elements in nature. He is voiced by Kenichi Suzumura in Japanese and Jason Liebrecht in English.

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Lenalee Lee is a very kind 16-year-old Exorcist from China. Her parents were killed by an akuma when she was very young. Due to her ability to use the Innocence, Lenalee was forced to become an Exorcist to use her strength. Because she was separated from her single, remaining family member at a young age, she went insane and had to be restrained due to repeated attempts at escape. During that time, she witnessed experiments involving implanting innocence into non-accommodators, and Rouvelier became a source of fear. However, her brother Komui joined the Order, easing her loneliness. Therefore, sanity restored, she fights for her brother as well as her friends as she knows she has a home to return. She has known Kanda and Lavi since they were young and met Allen at the beginning. She has grown a strong attachment to him throughout the series. Her perception of the "world" consists of her friends and family; whenever one of her friends dies, it seems to her as if a part of her world has been destroyed.

The Dark Boots her anti-akuma weapon, takes the form of a pair of black boots capable of high running speed, walking on water, and using sound waves as footholds. She invoked them beyond her ability and lost the ability to use her Innocence as well as most of her mobility. When she later drinks the liquefied form of the Innocence, the Dark Boots "evolved" from their equipment type into an entirely new crystal type that it is supposedly the first of this type. She is voiced by Shizuka Itō in Japanese and Luci Christian in English.

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Yu Kanda is a cold and rude 18-year-old Exorcist from Japan. He is the first Exorcist that Allen meets at the Black Order HQ and since then they have an ongoing loathing toward each other which often causes them declare a series of insults and offensive statements towards each other. He is a disciple of General Tiedoll and hates the fatherly way the man treats him. He is a Second Exorcist, a type of Exorcist created in the Synthetic Disciple Project Central forced onto the Chan and Epstein families nine years ago. Because of this, he can see lotus flowers blooming wherever he goes. As a child, there was only one and he was told it was an illusion. Since then, the flowers have multiplied.

In the anime adaption, the lotus flower is in an hourglass and is connected with his lifespan. As he approaches death, the flower loses its petals. He can recover much faster than ordinary humans due to a mysterious tattoo above his heart. Kanda refuses to die until he finds "a certain person".Originally forged by Zhu Chan, his anti-akuma weapon Mugen is an Innocence that originally took the form of a sleek chokuto and is later reforged as a katana. Mugen is capable of unleashing several techniques dubbed "illusions".He is voiced by Takahiro Sakurai in Japanese and Travis Willingham in English.

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Allen Walker is a soft-spoken and warm-hearted 15-year-old Exorcist of British origin and the main protagonist of the series. Allen was abandoned by his biological parents because of the paralysis and supposed "deformity" of his left arm and at age seven was adopted by Mana Walker. Three years later, Mana died and Allen turned him into an akuma, hoping him to be fully resurrected. Instead, he cursed Allen and sliced through his left eye, giving him the ability to detect disguised akuma. It was at this same moment that Allen’s left arm first awoke as an anti-akuma weapon and instinctively destroyed the akuma. He was later found by Cross Marian and trained as his disciple until he was sent to the Black Order headquarters five years later to officially become an Exorcist. His parasite-type anti-akuma weapon goes through two different forms resembling giant arms until it reaches its true form, the Crowned Clown which takes the form of a type of fur cape and a giant claw. Later on, it is able to additionally produce a large sword from Allen’s left arm, resembling the sword the Earl uses.

Shortly after his anti-akuma weapon takes the form of Crown Clown, his synchronization rate exceeded the percentage required for General level. Recently, allegations have arisen against Allen by Malcolm Rouvelier concerning recent suspicions that he may possess the implanted memories of the 14th Noah. These accusations are further exacerbated when Allen, upon impaling himself with the Crowned Clown, experiences severe pain, and starts to awaken the 14th Noah’s memories; he later bears a scar from this injury. When the Crown Clown is created, Allen claims his right hand is for the human race and his left is for the akuma. He is voiced by Sanae Kobayashi in Japanese and Todd Haberkorn in English.

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