At his alma mater of the Pontifical Roman Athenaeum S. Apoillinare, he was made professor of institutions and history of civil law in 1919, and later served as professor of Roman law for forty years. Within the Claretians, he held the posts of counselor of the Italian province, visitor to Germany, and general assistant to Italy, Central Europe, and China. He was appointed consultor, in the Roman Curia, of the Sacred Congregation of the Oriental Churches on 8 October 1929, and of the Sacred Congregation of Religious on 3 December of that same year.
Cardinal Larraona Saralegui was appointed Titular Archbishop of Diocaesarea in Isauria on 5 April 1962, and received his episcopal consecration on the following 19 April from Pope John, with Cardinals Giuseppe Pizzardo and Benedetto Aloisi Masella serving as co-consecrators, in the Lateran Basilica. He resigned as titular archbishop, on 20 April of that same year. Attending all four sessions of the Second Vatican Council, he served as a cardinal elector in the 1963 papal conclave that selected Pope Paul VI. Larraona Saralegui, who had acquired the reputation of being sternly conservative,[2] was cardinal protodeacon, or the most senior cardinal-deacon, from 26 June 1967 to 28 April 1969. He resigned as prefect of rites on 9 January 1968, and later exercised his right as a cardinal-deacon of ten years' standing to become a cardinal-priest (receiving the title of S. Cuore di Maria in the consistory of 28 April 1969).
Cardinal Larraona Saralegui died on 7 May 1973 at 10:10 am after a six-day bronchopulmonary infection in the Roman headquarters of the Claretians, at age 85. He is buried in the chapel of S. Giuseppe in the basilica of Sacro Cuore di Maria, according to his will.
While a priest, he also taught at the Pontifical Urbaniana University and the "Scuola Pratica" of the Sacred Congregation of Religious.
Larraona Saralegui prepared the particular law of his congregation at its general chapter in 1922.
He collaborated in the preparation of the apostolic constitutions "Provida Mater Ecclesia" of 2 February 1947; "Sponsa Christi" of 21 November 1950; and "Sedes Sapientiæ of 31 May 1956.
During his body's exposition in the chapel of Collegio Claretianum on Via Aurelia, visitors included the Pope, numerous cardinals and Curial officials, diplomats to the Holy See, and many Spanish priests and religious.
A street in Pamplona, the capital city of Navarre, is named after him.