In the 1957 edition of the Torneio Rio – São Paulo, he was one of the most important players as Flu were crowned champions without losing a game.

[1][2] He immediately moved to La Liga's Valencia CF, signing as a replacement for his compatriot Walter Marciano who had just died at the age of 29 in a car accident[4][5] after a friendly between the two sides.

[8] On 19 November 1961, Waldo scored four times in a 6–2 home rout of FC Barcelona,[9] and finished his first season abroad with 14 goals from 30 appearances.

On 12 June 1963, he equalised as Valencia came from behind to win 2–1 at GNK Dinamo Zagreb in the first leg of the Fairs Cup final (4–1 on aggregate).

[10] Waldo netted a career-best 24 league goals in the 1966–67 campaign,[11] and started in the 2–1 Spanish Cup final victory against Athletic Bilbao on 2 July 1967.