Waldo was born in Niterói, Rio de Janeiro. After joining Madureira Esporte Clube's youth setup in the early 1950s, he made his debuts as a senior in 1953.
On 11 April 1954 Waldo signed for Fluminense FC, being the top goalscorer of all tournaments which his team won. In the 1957 edition of the Torneio Rio – São Paulo, he was one of the most important players as Flu was crowned champions without losing one game.
Waldo left Fluminense on 1 July 1961 with a record of 314 goals in only 403 matches, being the club's top goalscorer of all time. He immediately moved to La Liga's Valencia CF, signing as a replacement to compatriot Walter Marciano who had just died at the age of 29 in a car accident after a friendly between the two sides.
Waldo made his debut in on 3 September 1961, in a 0–3 away loss against Real Zaragoza. Six days later he scored his first goals for the club, netting a brace in a 3–0 home win over Real Oviedo.
On 19 November, Waldo scored four times in a 6–2 home routing of FC Barcelona, 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).
Waldo netted a career-best 24 league goals in the 1966–67 campaign, also starting in the 2–1 Spanish Cup Final win against Athletic Bilbao on 2 July 1967. He represented the Che until 1970, scoring 157 goals in 294 games overall.
In the 1970 summer Waldo joined neighbours Hércules CF, retiring after one season in Segunda División at the age of 36.