Myron Healey
— John Dillinger (archive footage)
Paul Dubov
— Alvin Karpis
Sam Edwards
— Fred Barker
Richard Crane
— Homer Van Meter
Lyle Talbot
— Dr. William Guellfe, Plastic Surgeon
Jeanne Carmen
— Paula
Tamar Cooper
— Bonnie Parker
Baynes Barron
— Clyde Barrow
Doug Wilson
— Charles Arthur 'Pretty Boy' Floyd
Jim Davis
— Police Captain Stewart / Narrator
Sydney Mason
— Lieutenant Bill Baxter
Lash LaRue
— 'Doc' Barker
Ralph Moody
— Arthur 'Pa' Barker
Ann Morriss
— Mildred Jaunce - The Lady in Red
Aline Towne
— Shirley, Girl with Karpis
Regina Gleason
— Hope
Jeanne Bates
— Mrs. Ross Baxter
Jean Harvey
— 'Ma' Barker (archive footage)
Helen Van Tuyl
— Texas Lady Governor (archive footage)