Benfica when he was 15,[3] and was already an important first-team member just two years later, being part of the squads that won ten Primeira Liga championships and one European Cup.

[2] Simões moved to the United States at the age of 32, signing with the Boston Minutemen of the North American Soccer League.

After one season he moved to the Chicago Horizon, before finishing his career with the Kansas City Comets; he returned twice to his country during the off-season period, briefly representing G.D. Estoril Praia and U.F.C.I.

[7] He was dismissed in March 1984 and replaced by Ted Podleski, joining the Las Vegas Americans as assistant to Alan Mayer afterwards and also leaving in January 1985; in 1989, he was the SISL indoor season coach of the year with the Austin Sockadillos.

He was a member of the squad that finished third in the 1966 FIFA World Cup in England, scoring the first goal in the group stage opener against the same opponent (3–1 win).