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- Leonardo DiCaprio as J. Edgar Hoover
- Armie Hammer as Clyde Tolson
- Naomi Watts as Helen Gandy
- Josh Lucas as Charles Lindbergh
- Judi Dench as Anna Marie Hoover
- Dermot Mulroney as Norman Schwarzkopf, Sr.
- Damon Herriman as Bruno Richard Hauptmann
- Jeffrey Donovan as Robert F. Kennedy
- Ed Westwick as Agent Smith
- Zach Grenier as John Condon
- Ken Howard as Attorney General Harlan F. Stone
- Stephen Root as Arthur Koehler
- Denis O'Hare as Albert S. Osborn
- Geoff Pierson as A. Mitchell Palmer
- Lea Thompson as Lela Rogers
- Gunner Wright as Dwight D. Eisenhower
- Christopher Shyer as Richard Nixon
- Miles Fisher as Agent Garrison
- Jessica Hecht as Emma Goldman