Chrollo Lucilfer is the founder and leader of the Phantom Troupe, a notorious gang of thieves from Meteor City. His background is rooted in this lawless junkyard, a place discarded by society where he spent his childhood. Initially, he was a bright and kind child who participated in a theater group that dubbed foreign action shows for other children. A pivotal tragedy occurred when his friend Sarasa was kidnapped and brutally murdered by human traffickers. This event shattered the group's innocence and drove Chrollo to transform their acting troupe into a criminal organization. His goal was to make the Phantom Troupe so feared that outsiders would never again dare to harm the citizens of Meteor City. He and the other original members, including Uvogin, Machi, Phinks, Feitan, and Pakunoda, successfully tracked down and killed those responsible for Sarasa's death.

Physically, Chrollo is a young man of average height with black hair and dark eyes. His most distinctive features are a purple cross tattoo on his forehead and blue earrings he always wears. He typically styles his hair in a slicked-back undercut and dons a long black coat with an inverted cross on the back, though he may let his hair down and adopt a different look when gathering information discreetly.

Chrollo's personality is defined by a calm, analytical, and charismatic demeanor. He possesses a sharp intellect and remarkable powers of observation, often piecing together complex situations from minimal information. He displayed no fear when captured by Kurapika, instead calmly and methodically seeking to understand his captor's abilities. Despite his composed exterior, he is deeply emotional regarding his comrades. He shed tears upon learning of Uvogin's death through a prophecy and orchestrated a massacre of two thousand mafia members as a requiem to honor him. This duality shows he is a person who values deep emotional bonds but prioritizes the survival of the Spider, the entire Phantom Troupe, above all else, including his own life. He is an avid reader who is constantly surrounded by books. He follows a simple philosophy of stealing whatever he desires but discarding or selling it once his interest fades.

As the leader of the Phantom Troupe, Chrollo holds absolute authority, not through tyranny but through his unparalleled strategic mind and the respect he commands. He views the group as a living organism where he is merely the brain, a vital but not irreplaceable part. He famously stated that the survival of the Spider must come before the well-being of its head, his own life. Despite this philosophy, his members are fanatically loyal and consider his safety paramount. He is well-suited to assign tasks due to his deep understanding of each member's personality and abilities, although he tends to disappear on his own once a mission is complete.

Chrollo's role in the story is primarily that of an antagonist. He first gained infamy for leading the Troupe in a massacre of the Kurta clan to steal their unique red eyes, an act that created his archenemy, Kurapika. During the Yorknew City arc, he led the group in a heist to steal the Mafia's auction goods. After his comrade Uvogin was killed by Kurapika, the Troupe sought revenge, but Chrollo was ultimately captured by Kurapika. Kurapika sealed his Nen ability using a judgment chain, forcing him to go into exile to find an exorcist. His relationship with Hisoka Morow is another key dynamic. Hisoka, a fellow villain, joined the Troupe solely for the chance to fight and kill Chrollo. Chrollo eventually accepted the challenge, and after extensive preparation, he defeated Hisoka in a deadly battle at Heaven's Arena.

Chrollo's character has developed through his experiences. After having his Nen sealed, he demonstrated immense patience and strategic foresight, spending months, if not years, preparing for his rematch against Hisoka. This preparation led to a significant evolution in his combat abilities. Following the death of two of his members at Hisoka's hands, Chrollo's primary goal has shifted to a relentless pursuit of revenge against Hisoka, setting the stage for his involvement in the Succession Contest arc.

His notable abilities center on his Nen type, which is Specialist. His primary power is Skill Hunter, which manifests as a conjured book called Bandit's Secret. This ability allows him to steal another Nen user's ability and store it within its pages for his own use. To successfully steal an ability, he must fulfill several strict conditions: witnessing the ability in action, asking the user about it, having the user place their hand on the book's cover, and completing all this within one hour. To enhance this power, he developed a bookmark technique called Double Face. This allows him to use a stolen ability without holding the book open, and more critically, it enables him to use two different stolen abilities simultaneously. Among his most notable stolen abilities are Indoor Fish, which conjures man-eating fish that can only exist in a sealed room; The Sun and Moon, which creates explosive seals; and Order Stamp, which allows him to control puppets.