From 1965 to 1968 Berberian was committed to the San Francisco Opera, making his debut with the company in the title role of Béla Bartók's "Bluebeard's Castle" with Beverly Wolff as Judith and Gerhard Samuel conducting on May 25, 1965. Other roles he sang with the company included Alvise Badoero in "La Gioconda", Biterolf in Wagner's "Tannhäuser", The Bonze in "Madama Butterfly", both Charles V and the Friar in "Don Carlos", Ferrando in "Il trovatore", Inspector in "The Visitation", Narbal in Hector Berlioz's "Les Troyens", Orest's tutor in "Elektra", Pimen in "Boris Godunov", A rag picker in "Louise", Samuel in "Un ballo in maschera", The Speaker in "The Magic Flute", the Wise Man in "Christophe Colomb", and Man in the United States premiere of Kurt Weill's "Royal Palace".