Also in 1921, he appeared in a silent film of Don Juan Tenorio by the brothers Baños, which was shown the following year in New York City and Hollywood. He later directed his own Don Juan in 1924.

In 1927, he acted in Love of Sonya, directed by Albert Parker and starring Gloria Swanson. In 1932 he had small parts in Hollywood productions featuring Joan Bennett and Mary Astor. In the same period, he appeared in New York in several operas as well as the zarzuelas La Canción del Olvido ("The song of forgetting"), La Duquesa del Tabarín ("The Duchess of Tabarín"), Los Gavilanes, and La Montería. In 1934, he returned to Spain, where he had a major role in the film El Desaparecido ("The disappeared one") written and directed by Antonio Graciani. In 1935 he acted and sang in the film Poderoso Caballero ("A Big Guy"), directed by Màximo Nossik.

In 1936, with the outbreak of the Spanish Civil War, he returned to the United States, where he played the role of Captain Bill in a film called Capitán Tormenta, directed by Jules Bernhardt. A sequence of increasingly larger acting and singing roles mostly in English-language films followed, especially after 1940. Among his roles were Signor Matiste, Susan Alexander Kane's opera coach in Citizen Kane (1941); General Sebastiano in Five Graves to Cairo (1943); Don Miguel in The Black Swan (1942); Fernando in For Whom the Bell Tolls (1943); Sam Garlopis in Double Indemnity (1944); and a singing Christopher Columbus in Where Do We Go From Here?. He continued for the next several decades in a miscellany of character roles.

Bonanova was also an uncredited technical consultant for the film Blood and Sand (1941), and produced and appeared in the Spanish-language film La Inmaculada (a name of the Virgin Mary, "Immaculate")(1939).

Bonanova played the father of twins Esther Williams, and Ricardo Montalbán in the 1947 film Fiesta. In 1949, Bonanova collaborated with Ambrose Barker (a former music hall performer who had, with his partner/wife, Peggy Wynne, had some success on the British colonial circuit in the 1920s–1930s) on a musical entitled "Glamor/Glamour is the Gimmick." It got bad reviews—what may have been popular and witty in the early 1930s didn’t make it in 1949.

In the 1950s, he appeared in an episode of I Love Lucy as a fake psychic who uses his stage apparatus to make it appear as though Lucy is able to speak Spanish to her mother-in-law.

In 1952, he played an Italian opera singer, Anthony Branchetti, in the 4th episode of My Little Margie where Margie helps her father by convincing Mr. Branchetti to appear at a party in his honor to impress a reluctant client of Honeywell & Todd.

In 1953 he played Lou Costello's Uncle Bozzo in the Abbott & Costello episode of "Uncle Bozzo's Visit."

Bonanova died in 1969 in Woodland Hills, California of a cerebral hemorrhage and is buried at Holy Cross Cemetery in Culver City, California.