Gayarre sang a broad repertoire, ranging from bel canto works to the earlier music-dramas composed by Wagner. In the 1870/71 season, at the Teatro Regio di Parma, he sang with great success in a trio of Verdi operas, "I Lombardi alla prima crociata", "Un ballo in maschera" and "Rigoletto". In October 1872 at the Teatro Comunale di Bologna, he sang Amenophis in Rossini's "Moïse et Pharaon". Only a month later, he sang the title role in Wagner's Tannhäuser there, its first performance in Italy. Gayarre's other great Wagnerian role was "Lohengrin" which he sang in its first ever performance at the Teatro Real in Madrid in 1881. However, the following year he was back in the bel canto repertoire with performances of "I puritani" and "La favorita" at Valladolid's Teatro Calderón. Gayarre was also a noted interpreter of the French repertoire including Gounod's "Faust" and Meyerbeer's "Les Huguenots", "Le prophète" and "L'Africaine".