- Ralph Fiennes as Monsieur Gustave H., the Grand Budapest Hotel's renowned concierge
- Tony Revolori as Zero Moustafa, the newly hired bellhop mentored by Gustave
- F. Murray Abraham as the elderly Zero
- Adrien Brody as Dmitri Desgoffe-und-Taxis, Madame D.'s son
- Willem Dafoe as J. G. Jopling, a ruthless hitman working for Dmitri
- Saoirse Ronan as Agatha, an apprentice baker and Zero's love interest
- Tilda Swinton as Dowager Countess Céline Villeneuve Desgoffe-und-Taxis, known as Madame D., a wealthy dowager countess and the secret owner of the hotel
- Edward Norton as Albert Henckels, the police investigator of Madame's murder
- Mathieu Amalric as Serge X, a shifty butler who works for Madame D
- Jeff Goldblum as Deputy Vilmos Kovacs, the lawyer representing Grand Budapest interests
- Harvey Keitel as Ludwig, leader of a prison gang at Checkpoint Nineteen
- Tom Wilkinson as Author, writer of The Grand Budapest Hotel
- Jude Law as the young Author in 1968
- Bill Murray as M. Ivan, Gustave's friend and one of several concierges affiliated with the Society of the Crossed Keys
- Jason Schwartzman as M. Jean, the Grand Budapest's concierge in 1968
- Owen Wilson as M. Chuck, a Society of the Crossed Keys concierge
- Léa Seydoux as Clotilde, maid at Schloss Lutz
Other cast members included Larry Pine as Mr. Mosher, Milton Welsh as Franz Müller, Giselda Volodi as Serge's sister, Wolfram Nielacny as Herr Becker, Florian Lukas as Pinky, Karl Markovics as Wolf, Volker Michalowski as Günther, Neal Huff as Lieutenant, Bob Balaban as M. Martin, Fisher Stevens as M. Robin, Wallace Wolodarsky as M. Georges, Waris Ahluwalia as M. Dino, Jella Niemann as the young woman, and Lucas Hedges as a pump attendant.
