He represented Agra University in 1954–55 and a year later won the Obaidullah Gold Cup Hockey Championship.

Gurbux Singh first played for East Bengal Club in 1957, and was influential in their first victory at the Beighton Cup that year.

By 1963, he was made captain, and led the team that won the gold medal at the 1964 Tokyo Olympics and the 1966 Bangkok Asian Games.

In the 1968 Mexico City Olympics, he shared captaincy with Prithipal Singh, where India won the bronze medal.

In 2013, he received the Banga Bibhushan, a title instituted by the West Bengal government to honour distinguished achievements in various fields.