- Myron Healey
- John Dillinger
- Jean Harvey
- 'Ma' Barker
- Paul Dubov
- Alvin Karpis
- Sam Edwards
- Fred Barker
- Richard Crane
- Homer Van Meter
- Tamar Cooper
- Bonnie Parker
- Baynes Barron
- Clyde Barrow
- Doug Wilson
- Charles Arthur 'Pretty Boy' Floyd
- Jim Davis
- Police Captain Stewart / Narrator (archive footage)
- Lyle Talbot
- Dr. William Guellfe, Plastic Surgeon
- Sydney Mason
- Lieutenant Bill Baxter
- Lash LaRue
- 'Doc' Barker
- Ralph Moody
- Arthur 'Pa' Barker
- Jeanne Carmen
- Paula
- Ann Morriss
- Mildred Jaunce - The Lady in Red
- Aline Towne
- Shirley, Girl with Karpis
- Regina Gleason
- Hope
- Jeanne Bates
- Mrs. Ross Baxter
- Helen Van Tuyl
- Texas Lady Governor
- Knobby Schaeffer
- Adam Richetti
- Russell Whitney
- Verne Miller
- Coulter Irwin
- FBI Agent Ross Baxter
- Robert Kendall
- Baby Face Nelson
- Sam Flint
- FBI Chief
- Bill Baldwin
- Special Agent Fenton / Narrator
- Robert Bice
- FBI Agent Tyler
- William Boyett
- FBI Agent on Pier
- Ray Boyle
- Raymond Hamilton
- Scott Douglas
- FBI Agent Clifton
- Darlene Fields
- Connie, Dillinger's Girl
- Dick Foote
- Prison Trustee
- Texas Joe Foster
- Tony Milento
- Joseph J. Greene
- Arthur Troser
- Billy Griffith
- Bucher
- Frank Hamer
- Self (Texas Ranger)
- Harold 'Tommy' Hart
- Garageman
- Percy Helton
- Pool Room Proprietor
- Glenn Holden
- Dillinger's Jail Guard
- Florence Lake
- Bessie, the Landlady
- Hank Patterson
- Scully Wass (Farmer)
- Robert Vanselow
- John Hamilton
- Smoki Whitfield
- The Bootblack
