Best known for his leading part in the Evaton bus boycott of 1955 to 1956. He was born in 1930 in Winburg in the Orange Free State and attended St Peter's Secondary School in Johannesburg, matriculating in 1948. While studying medicine at the University of the Witwatersrand in the early 1950s, he was caught up in the activities of the Transvaal Youth League and abandoned his studies to become a full-time political organizer at the time of the 1952 Defiance Campaign.

The Evaton bus boycott, during which African bus authorities were forced to cancel a fare increase owed much of its success to the efforts of Molefi and Vusi Make. From 1956 until 1961 he was a defendant in the Treason Trial, becoming one of the few defendants to identify with the Pan Africanist Congress after its founding in 1959.

In December 1960 he and ZB Molete represented the PAC at the consultative conference of African leaders in Johannesburg. In late 1961, Molefi fled to Basutoland, where he joined the PAC executive committee in exile. He later became a press correspondent, covering Lesotho for several South African newspapers. Attempts by the Lesotho government to deport him in the late 1960s were eventually discontinued.

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