Allen Walker
An Exorcist of British origin and the main protagonist of the series. Allen was abandoned by his biological parents because of the supposed "deformity" of his left arm and later adopted by Mana Walker. At some moment, Mana died and Allen turned him into an Akuma, hoping him to be fully resurrected but instead, he cursed Allen and sliced through his left eye. It was at this same moment that Allen's left arm first awoke as an anti-Akuma weapon and instinctively destroyed the Akuma.

Lenalee Lee
Komui's younger sister, and the assistant Head Officer, Lenalee is a 16-year-old Exorcist from China. Her parents were killed by an Akuma when she was very young. She feels guilty for imprisoning Komui at the Headquarters (in that he threw everything away for her sake). She explains to Allen that 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. She has a strong sense of friendship, and constantly worries about her friends and gets mad at them if they overextend themselves. Although she cherishes all of her friends dearly, she appears to care deeply about Allen, in particular.

Lavi
A cheerful red-haired Exorcist of mixed race, who aims to become a Bookman and is working along the Black Order just to be close to the events that must be seen. It was also revealed that Lavi was once cold and indifferent to others, for a Bookman only lives to view and record history and that humans are nothing more than 'ink' on a page. However, over time Lavi's personality changed and he began to truly care about others, slowly casting aside his identity as a Bookman as shown when he thought that Allen was killed by Tyki Mikk he tried to avenge Allen by attempting to kill Tyki himself.

Yu Kanda
He has a harsh tongue, a foul mouth, and a cold manner, and tends to say "che" a lot. His master, General Tiedoll, calls him "an antisocial humbug." However, it is clear that Kanda does care for his fellow Exorcists and the Finders (whom he claims not to care about). For example, he saves Allen from an Akuma (despite his own injuries) even though he said earlier that he would not help Allen even if Allen were about to die. He also rescues Gozu, a Finder who accompanies him on several missions. He masks his emotions and often claims, "It's none of my business."

Miranda Lotto
A woman whose clock caused time to rewind in her town, which started when she was able to connect to the Innocence within the clock. Miranda is German, and twenty-five years old. She often feels inferior and useless, which caused her to be fired from all one hundred jobs she tried to work in. This contributes to her chronic depression. With the help of Allen and Lenalee, she became determined to be a useful Exorcist. Her weapon is a disk called "Time Record", located on her right arm. When activated, it appears from her right arm and "slides" to her wrist. The disk has two green, glowing circles, with circles orbiting the center.

Arystar Krory
A Romanian with split personalities: a soft, kind, and overly-emotional "normal" side, and an aggressive, cocky, "battle-mode" side. For his entire life, Krory lived in a secluded castle. Because of the way he attacked villagers, drinking their blood and then carrying them off, and because of his stereotypical vampire theme, he was believed to be a vampire by the surrounding villagers and shunned. The true reason for this behavior was his teeth, made of Innocence, that caused him to instinctively attack Akuma, though the villagers and Krory (before meeting Allen and Lavi) did not know this. Later, he fell in love with a woman named Eliade, unaware of the fact that she was actually an Akuma. After Allen and Lavi come across the village and their "vampire problem" during their search for Cross, they realize that Krory has innocence, and recruit him as an Exorcist.