- Will Ferrell as Harold Crick, an IRS agent who starts hearing Eiffel's voice narrating his life
- Maggie Gyllenhaal as Ana Pascal, a baker who is being audited by Crick and begins to fall in love with him
- Emma Thompson as Karen Eiffel, an author known for killing the protagonists in her novels, but has been suffering from writer's block
- Dustin Hoffman as Professor Jules Hilbert, a literature expert advising Crick
- Queen Latifah as Penny Escher, an assistant who helps authors finish their works
- Tony Hale as Dave, Crick's friend from his work
- Tom Hulce as Dr. Cayly
- Linda Hunt as Dr. Mittag-Leffler, a psychologist whom Crick sees in hopes of solving his narration problem
- Kristin Chenoweth as Book Channel Host
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