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Johnny Depp as John Dillinger: An American bank robber whose exploits dominated the press during what is sometimes referred to as the public enemy era, between 1931 and 1935.
Christian Bale as Melvin Purvis: An FBI agent chosen by J. Edgar Hoover to lead a manhunt to catch Dillinger.
Marion Cotillard as Billie Frechette: Dillinger's torch singer girlfriend.
Channing Tatum as Pretty Boy Floyd: An American bank robber and alleged killer.
Giovanni Ribisi as Alvin Karpis: A noted criminal in the United States known for his alliance with the Barker gang in the 1930s. He was the last "Public Enemy" to be captured.
Stephen Dorff as Homer Van Meter: A criminal and bank robber active in the early 20th century, most notably as a criminal associate of Dillinger and Baby Face Nelson.
Billy Crudup as J. Edgar Hoover: The first Director of the Federal Bureau of Investigation (FBI) of the United States.
Leelee Sobieski as Polly Hamilton: Dillinger's final girlfriend, ignorant of his true identity.
Jason Clarke as John "Red" Hamilton: A Canadian criminal and bank robber active in the early 20th century, most notably as a criminal associate of Dillinger.
John Ortiz as Frank Nitti: Al Capone's right-hand man and Underboss in the Chicago Outfit.
David Wenham as Harry Pierpont: A member of Dillinger's crew.
Stephen Graham as Baby Face Nelson[7]: He was a bank robber who acquired his moniker, Baby Face Nelson due to his youthful appearance and small stature. After Dillinger's death in July 1934, Nelson became Public Enemy Number One.
Richard Short as Samuel P. Cowley: He was the FBI agent who brought down Baby Face Nelson but was mortally wounded in the gunbattle in Barrington, Illinois.
Christian Stolte as Charles Makley: A known associate of Dillinger's and who broke him out of prison in 1933. By the end of that year, Makley ranked fourth on Illinois' list of "public enemies", behind Dillinger, Pierpont, and Hamilton.
Stephen Lang as Charles Winstead: He is the leader of the Texas Rangers who join the manhunt for Dillinger and his gang.
Shawn Hatosy as John Madala: An FBI agent who helped capture Ma Barker.
Branka Katic as Anna Sage: the infamous "Lady in Red" who was romantically involved with Dillinger at the time of his murder.
Emilie de Ravin as Anna Patzke: a bank teller who was taken hostage by Dillinger and later released.
James Russo as Walter Dietrich: a man who Dillinger met while in the Michigan City penitentiary. He taught Dillinger and others "the methods of Herman 'Baron' K. Lamm, a Prussian army officer turned highly successful bank robber".
Lili Taylor as Sheriff Lillian Holley: Sheriff of Lake County Jail, Crown Point, Indiana, where Dillinger was incarcerated