Levine was a member of the notorious Mafia gang, Murder, Inc., and is credited with being the trigger man, with Dutch Schultz lieutenant Abraham "Bo" Weinberg, in the 1931 murders of Joe "The Boss" Masseria and, along with Joe Adonis, Albert "The Mad Hatter" Anastasia and Benny "Bugsy" Siegel, one of the three hitmen sent by Meyer Lansky to assassinate the Sicilian Mafia boss Salvatore Maranzano in his office.

In his court testimony, Abe Reles recalled that Levine once complained to him that "any time I've got a contract Charlie is around to do the killing."

A portrait of the seldom-photographed Levine appears in the book New York City Gangland, depicting him during his career as a Murder, Inc.

One of them, Red Levine, was reputed to have been one of the assassins of Salvatore Maranzano, the old-school mobster who helped to found America's Cosa Nostra.

Law enforcement officials, as well as longtime union members and mob associates (often the same thing in the NMDU) say that Levine cleverly allowed each of the city's five Mafia families to have a piece of the newspaper delivery action, which included bootleg sales of stolen papers as well as loan-sharking and gambling among drivers.

"[7] In his later years, Levine reportedly spent time in the Little Italy district, frequenting the Knotty Pine Social Club, a known Mafia hangout operated by Genovese capo Peter DeFeo, as well as the Raven Knights Social club, more commonly known in later years as the "Ravenite".