1961 marked a turning point in Rey's career when he made his first film for the iconoclastic and internationally renowned Luis Bunuel; the result was one of the finest films of the actor's career, "Viridiana" (1961). As the dense but somewhat nasty and always lustful uncle, Don Jaime, Rey enjoyed one of his best-remembered roles, relentlessly pursuing the eponymous heroine, a novice nun. Rey eventually racked up more than 150 feature credits, working for directors including Orson Welles ("Chimes at Midnight" 1966, excellent as Northumberland), Maurice Cloche ("The Viscount" 1967), Alberto Lattuada ("Bianco, Rosso e../White Red and.." 1971), Lina Wertmuller ("Seven Beauties" 1975), Vincente Minnelli ("A Matter of Time" 1976), Robert Altman ("Quintet" 1979), and Stephen Frears ("The Hit" 1984). Rey's work in Carlos Saura's "Elisa, mia vida" (1977) won him best actor honors at Cannes.
Usually sporting his trademark goatee, Rey possessed an aristocratic dignity which suited roles from statesmen to priests and made him ideal for historical sagas; one of his last films was Ridley Scott's misfire Columbus biopic, "1492: The Conquest of Paradise" (1992) and that same year, Rey enjoyed considerable acclaim in a Spanish TV miniseries as Don Quixote. In features Rey often portrayed urbane, cynical men weary of life. He reunited with Bunuel for three more films in the 70s, in which the witty master director would exploit Rey's expressive deadpan in roles as corrupt or dirty old men. He again corrupted a young woman (Catherine Deneuve) in the pensive yet deliciously perverse "Tristana" (1970), brought both class and wickedness to his ambassador in his award-winning performance in the witty "The Discreet Charm of the Bourgeoisie" (1972) and again endured sexual frustration as he pursued a woman (played by two different actresses) in Bunuel's last film, "That Obscure Object of Desire" (1977). American audiences, however, probably still remember Rey best as the crafty drug lord Charnier in "The French Connection" (1971) and its 1975 sequel.