In 1869, shortly after commencing his studies in Milan, Gayarre made his operatic debut as Nemorino in L'elisir d'amore in Varese. Particularly renowned for his interpretation of Fernando in "La Favorita", he was also considered by critics of the time, especially in Italy, to be an excellent actor with a commanding stage presence. Gayarre's earliest successes and fame came from his performances in the major opera houses of Italy, where he created the role of Marcello in "Il Duca d'Alba" in 1871 and Enzo in the 1876 premiere of "La Gioconda". However, he was soon highly in demand in Paris and London as well as his native Spain. Gayarre also sang in Lisbon, Vienna and Saint Petersburg and toured Brazil and Argentina with the Spanish contralto Elena Sanz, a frequent stage partner, especially at La Scala. Towards the end of his career, in 1887, he sang Sobinin in the first London performance of Glinka's "A Life for the Tsar".