Jair moved to Italian side Internazionale in November 1962, and went on to play a total of 260 senior games for the Milan club in two spells (1962–1967 and 1968–1972). He was notably a key member of Helenio Herrera's "Grande Inter" squad on the right wing, and won four Serie A titles (two of which were won consecutively), and two European Cups in 1964 and 1965, as well as consecutive Intercontinental Cups in 1964 and 1965, during his time at the club.