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More serious roles he recorded include the King of Egypt in two recordings of Aida with Renata Tebaldi, Mathieu in Andrea Chénier, also with Tebaldi, two recordings of the Bonze in Madama Butterfly with both Anna Moffo and Leontyne Price, and the Gessler in Rossini's Guglielmo Tell (William Tell) with Giuseppe Taddei and Rosanna Carteri.
Tozzi was the recipient of three Grammy Awards: in 1960 the Grammy Award for Best Classical Performance, Operatic or Choral for The Marriage of Figaro with Erich Leinsdorf; in 1961 the Grammy Award for Best Opera Recording for Puccini's Turandot, with Erich Leinsdorf; and in 1963 the Grammy Award for Best Opera Recording for Georg Solti's recording of Verdi's Aida (with Leontyne Price and Jon Vickers).
In 1963, in a studio recording of Porgy and Bess featuring Leontyne Price and William Warfield, he performed Sportin' Life's two main arias from the opera, "It Ain't Necessarily So" and "There's A Boat Dat's Leavin' Soon For New York".
One of his final recordings was the Verdi Requiem conducted by Fritz Reiner for Decca Records which was recorded as late as June 1960 with Leontyne Price, Rosalind Elias and Giorgio Tozzi.
Some of the celebrated opera singers featured on Live from the Met have included Plácido Domingo, Luciano Pavarotti, Beverly Sills, Samuel Ramey, Renée Fleming, Joan Sutherland, Marilyn Horne, Renata Scotto, Leontyne Price, and Sherrill Milnes.
Among the opera companies and stars who have appeared at Symphony Hall are the Metropolitan Opera, Jerome Hines, Beverly Sills, Roberta Peters, Leontyne Price, and Robert Merrill (who made his debut there).
He was also involved in the early career development of such singers as Leontyne Price, George London and Mario Lanza.
On September 16, 1966 he appeared as the Sentinel in the world premiere of Samuel Barber's Antony and Cleopatra for the opening of the new Metropolitan Opera House with Leontyne Price as Cleopatra and Justino Díaz as Anthony.