The Crimebusters (1961)

Nicholas Cain (Peter Mark Richman), a former high-level mob lawyer who decides to leave the criminal underworld. Seeking redemption, he becomes a federal government agent with a singular mission: to bring down the nation's 100 most dangerous and influential organized crime figures. The film depicts the specialized government agents as they hunt these high-profile crooks, focusing on Cain's personal crusade to dismantle the very syndicates he once protected. Based on the "Cain's Hundred" TV series.