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Žujović first joined the Communist Party of Yugoslavia (KPJ) at the age of 25 in 1924 in Belgrade, and worked as an organizer there before becoming a secretary of the party. When the communists became a threat to the Kingdom of Yugoslavia, he was arrested and released but kept under surveillance by the police. In 1933 Žujević left the Kingdom of Yugoslavia for the USSR where he became a recipient of a Communist scholarship in the Comintern school. Among the students at the school were his Belgrade colleagues, Rodoljub Čolaković and Milan Gorkić, the KPJ's general secretary, who in 1936 was summoned to Moscow from Paris and upon his arrival was deposed and jailed in Lubyanka, only to be executed the following year.
Sreten Žujović was a member of Yugoslav delegation at a United Nations Conference on International Organization. The delegates drew up the 111-article Charter, which was adopted unanimously on 25 June 1945 in the San Francisco Opera House.