This "best remembered" of all the crime stoppers shows was billed as "the only national program that brings you authentic police case histories." It premiered on January 15, 1936, and was broadcast over 21 years through November 27, 1957.Gang Busters aired on CBS from January 15, 1936 to June 15, 1940, sponsored by Colgate-Palmolive and Cue magazine. From October 11, 1940 to December 25, 1948, it was heard on the Blue Network, with various sponsors that included Sloan's Liniment, Waterman pens and Tide. Returning to CBS on January 8, 1949, it ran until June 25, 1955, sponsored by Grape-Nuts and Wrigley's chewing gum. The final series was on the Mutual Broadcasting System from October 5, 1955 to November 27, 1957.

Gang Busters often featured prominent names in radio broadcasting, many of whom also starred in movies and television. Two of the most famous were Richard Widmark and Art Carney. Widmark was typecast as a villain for many years, but finally managed to break that mold. Carney became especially famous for his role with Jackie Gleason on The Honeymooners, but he had a much broader career than that. Joan Banks, who later played many TV roles, was a regular cast member. Her husband, Frank Lovejoy, also appeared often, and later went on to star in many movies and an ABC crime drama. Larry Haines was another regular on the show. He went on to an extensive career in TV soap operas. A lesser known actor on the show was Leon Janney, who apparently played both juvenile roles and ones requiring an unusual accent.