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Although Robbins pushed for 29-year-old Carol Lawrence, the first Maria, to be cast in the same role in the film, after seeing her screen test the producers agreed she was too old to play the part. Tony Mordente, who played A-Rab on stage, was cast as Action in the film, and George Chakiris, Riff in the London stage production, played Bernardo in the film. Tucker Smith, who joined the Broadway production several months into its run, played Diesel, renamed Ice for the film. David Winters, the first stage Baby John, played A-Rab, Eliot Feld, an ensemble member and understudy for Baby John on Broadway, played Baby John. Jay Norman, Juano on stage, appeared as Pepe. Reprising their stage roles in the film were Carole D'Andrea as Velma, Tommy Abott as Gee-Tar, and William Bramley as Officer Krupke.

Elvis Presley was approached for Tony, but his manager, Colonel Tom Parker, turned down the part. Others who were considered for the part included Tab Hunter, Russ Tamblyn , Warren Beatty, Burt Reynolds, Richard Chamberlain, and Robert Redford.

Hunter, then 30, and Reynolds, then 25, were considered for the part due to their Broadway and singing credits, but they were dismissed because of their age. Reynolds was also considered "too tough" for the part. Chamberlain was believed to be "too mature" for the role. Tamblyn impressed producer Robert Wise, and was given the supporting role of Riff. Ultimately, Richard Beymer won the part of Tony.

Natalie Wood was filming Splendor in the Grass with Warren Beatty and was romantically involved with him off-screen. The producers were not considering her for the role of Maria at that time. When considering Beatty for the role of Tony, Robert Wise requested a reel of his work. However, after seeing a clip from Splendor in the Grass, the producers decided his co-star Wood was perfect for Maria, but Beatty was not suitable for the role of Tony.

Jill St. John, Audrey Hepburn, Diane Baker, Jane Fonda, Elizabeth Ashley, and Suzanne Pleshette were among the many actresses who were considered for the role of Maria in the film.