- Leonardo DiCaprio as Edward "Teddy" Daniels / Andrew Laeddis (both U.S. Marshals)
- Mark Ruffalo as Chuck Aule / Dr. Lester Sheehan, Teddy's primary psychiatrist
- Ben Kingsley as Dr. John Cawley, senior psychiatrist at the hospital
- Max von Sydow as Dr. Naehring, psychiatrist
- Michelle Williams as Dolores Daniels, Teddy's manic-depressive wife
- Emily Mortimer as Rachel 1 / a nurse helping in the role-play
- Patricia Clarkson as Rachel 2
- Jackie Earle Haley as George Noyce, a patient in Ward C
- Ted Levine as Warden
- John Carroll Lynch as Deputy Warden McPherson
- Joseph Sikora as Glen Miga
- Elias Koteas as Laeddis, the fictional arsonist
- Robin Bartlett as Bridget Kearns
- Christopher Denham as Peter Breene
- Curtiss Cook as Trey Washington
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