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- Ralph Fiennes as Monsieur Gustave H.
- Tony Revolori as Young Zero Moustafa
- Adrien Brody as Dmitri Desgoffe und Taxis
- Willem Dafoe as J.G. Jopling
- Jeff Goldblum as Deputy Vilmos Kovacs
- Saoirse Ronan as Agatha
- Edward Norton as Inspector Henckels
- F. Murray Abraham as Old Zero Moustafa
- Mathieu Amalric as Serge X.
- Jude Law as The Author as a Young Man
- Harvey Keitel as Ludwig
- Bill Murray as Monsieur Ivan
- Lea Seydoux as Clotilde
- Jason Schwartzman as Monsieur Jean
- Tilda Swinton as Madame Celine Villeneuve Desgoffe und Taxis
- Tom Wilkinson as The Author as an Old Man
- Owen Wilson as Monsieur Chuck
- Bob Balaban as M. Martin