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The Sheik

After quitting Metro, Valentino took up with Famous Players–Lasky, forerunner of the present-day Paramount Pictures, a studio known for films that were more commercially focused. Mathis soon joined him, angering both Ivano and Rambova.

Jesse L. Lasky intended to capitalize on the star power of Valentino, and cast him in a role that solidified his reputation as the "Latin lover". In The Sheik (1921), Valentino played the starring role of Sheik Ahmed Ben Hassan. The film was a major success and defined not only his career but his image and legacy. Valentino tried to distance the character from a stereotypical portrayal of an Arab man. Asked if Lady Diana (his love interest) would have fallen for a "savage" in real life, Valentino replied, "People are not savages because they have dark skins. The Arabian civilization is one of the oldest in the world... the Arabs are dignified and keen-brained."

Famous Players produced four more feature-length films over the next 15 months. His leading role in Moran of the Lady Letty was of a typical Douglas Fairbanks nature; however, to capitalize on Valentino's bankability, his character was given a Spanish name and ancestry. The film received mixed reviews, but was still a hit with audiences.

In November 1921, Valentino starred alongside Gloria Swanson in Beyond the Rocks. The film contained lavish sets and extravagant costumes, though Photoplay magazine said the film was "a little unreal and hectic." Released in 1922, the film was a critical disappointment. Years after its release, Beyond the Rocks was thought to be lost, save for a one-minute portion. But in 2002, the film was discovered by the Netherlands Film Museum. The restored version was released on DVD in 2006.

In February, 1922 Life magazine reported that, according to the Famous Players press office, Valentino would henceforth be known as "Rodolph" rather than "Rudolph."

In 1922, Valentino began work on another Mathis-penned film, Blood and Sand. He played the lead— bullfighter Juan Gallardo—and co-starred with Lila Lee and Nita Naldi. Initially believing the film would be shot in Spain, Valentino was upset to learn that the studio planned on shooting on a Hollywood back lot. He was further irritated by changes in production, including a director of whom he did not approve.

After finishing the film, Valentino married Rambova, which led to a bigamy trial, as he had been divorced from his first wife, Jean Acker, for less than a full year, as required by California law at the time. The trial was a sensation and the pair was forced to have their marriage annulled and to be separated for a year. Despite the trial, the film was still a success, with critics calling it a masterpiece on par with Broken Blossoms and Four Horsemen. Blood and Sand became one of the four top-grossing movies of 1922, breaking attendance records, and grossing $37,400 at the Rivoli Theatre alone. Valentino considered this one of his best films.

During his forced break from Rambova, the pair began working separately on the Mathis-penned The Young Rajah. Only fragments of this film, recovered in 2005, still remain. The film did not live up to expectations and underperformed at the box office. Valentino felt he had underperformed in the film, being upset over his separation with Rambova. Missing Rambova, Valentino returned to New York after the release of The Young Rajah. They were spotted and followed by reporters constantly. During this time, Valentino began to contemplate not returning to Famous Players, although Jesse Lasky already had his next picture, The Spanish Cavalier, in preparation. After speaking with Rambova and his lawyer Arthur Butler Graham, Valentino declared a 'one-man strike' against Famous Players.