- Johnny Depp John Dillinger
- Christian Bale Melvin Purvis
- Marion Cotillard Billie Frechette
- Billy Crudup J. Edgar Hoover
- Stephen Dorff Homer Van Meter
- Stephen Lang Charles Winstead
- John Ortiz Phil D'anddrea
- David Wenham Harry "Pete" Pierpont
- Stephen Graham Nelson Cara de Niño
- Giovanni Ribisi Alvin Karpis
- Jason Clarke John "Red" Hamilton
- Rory Cochrane Agente Carter Baum
- Channing Tatum Floyd El Guaperas
- Emilie de Ravin Anna Patzke
- Lili Taylor Sheriff Lillian Holley
- Shawn Hatosy John Madala
- Matt Craven Gerry Campbell
- Leelee Sobieski Polly Hamilton
- Branka Katic Mujer de rojo
- Bill Camp Frank Nitti
- Christian Stolte Charles Makley
- Spencer Garrett Tommy Carroll
- Carey Mulligan Carol Slayman
- Laurence Mason
- Domenick Lombardozzi Gilbert Catena
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