In 1966, Caballé made her first appearance with the Philadelphia Lyric Opera Company as Maddalena di Coigny in Giordano's "Andrea Chénier" and her Italian debut at the Maggio Musicale Fiorentino as Leonora in Verdi's "Il trovatore", followed by Bellini's "Il pirata" in 1967. She returned to Philadelphia in 1967 to sing the title roles in Puccini's "Tosca" and "Madama Butterfly", and to the Met to sing three Verdi heroines: Leonora alongside Richard Tucker as Manrico in "Il Trovatore", Desdemona in "Otello" with James McCracken in the title role, and Violetta in "La traviata", with Tucker and George Shirley alternating as Alfredo. She returned to the Met the following year in the title role in Verdi's "Luisa Miller", and in 1969 for the role of Liù in Puccini's "Turandot", with Birgit Nilsson in the title role and James King as Calàf. She also returned to Philadelphia as Imogene in Bellini's "Il pirata" (1968) and Lucrezia Borgia (1969).