In 1959 he signed with Real Zaragoza from local Racing de Ferrol, going on to remain with the former club until his retirement 11 years later.

[1] During his spell with the Aragonese, always spent in La Liga, Marcelino scored 117 goals in all competitions, contributing solidly as they won three major titles, including two Copa del Rey trophies.

[2] He was part of an efficient attacking line dubbed Los Magníficos (The Magnificent) which also featured Canário, Carlos Lapetra, Eleuterio Santos and Juan Manuel Villa.

[4][5] In the former tournament, he scored the decisive 2–1 in the final against the Soviet Union, through a header.

[6] At the time of his debut, Marcelino was the first Zaragoza player to ever represent the national team.