He is best known for his roles in four Spaghetti Western films: Ramón Rojo in Sergio Leone's A Fistful of Dollars (1964), El Indio in Leone's For a Few Dollars More (1965), El Chuncho Munoz in Damiano Damiani's A Bullet for the General (1966) and Professor Brad Fletcher in Sergio Sollima's Face to Face (1967).

He is also recognized for his performances in Jean-Pierre Melville's Le Cercle Rouge (1970), Giuliano Montaldo's Sacco & Vanzetti (1971) and Giordano Bruno (1973), and Francesco Rosi's Christ Stopped at Eboli (1979).

[3] His mother, Carolina Bianchi, belonged to a wealthy Milanese industrial family, and his younger brother Claudio was an actor as well.

[3] He went to Rome to train for an acting career at the Accademia Nazionale di Arte Drammatica Silvio D'Amico, obtaining a degree in 1957.

[6] 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.

[1] Volonté's performances as memorable but neurotic characters, or as a gifted leader of brigands or revolutionaries, together with the unexpected, worldwide success of the films, gave him international fame.

Volonté had already played comedies, including A cavallo della tigre (1961) by Luigi Comencini,[1] and confirmed his versatility in L'armata Brancaleone (1966).