Volonté made his debut in 1960 in Sotto dieci bandiere, directed by Duilio Coletti. Just four years later, he played "Ramón Rojo" in A Fistful of Dollars (1964), and "El Indio" in For a Few Dollars More (1965), both for cash reasons as he did not consider either role serious. Both films were directed by the then-unknown Sergio Leone, and Volonté's roles in them would bring him his greatest recognition from American audiences. He played Carlo Levi in Cristo si è fermato a Eboli (1979), which was based on Levi's autobiographical account of his years in internal-exile in Aliano, south Italy, in the 1930s. The English title is Christ Stopped at Eboli. Volonté played the memorable role of the Bandito-turned-guerrilla, El Chucho, in A Bullet for the General (1966).