In an open letter seen today, Ahmed Kathrada, 86, joined a growing chorus of leading figures calling for Zuma to leave office.
The criticism comes after the Constitutional Court on Thursday found Zuma in breach of the constitution for using public funds to upgrade his private home at Nkandla village.
Zuma, who has long denied wrongdoing for the work valued in 2014 at 216 million rand (then USD 24 million), yesterday apologised to the nation for the misuse of public funds.
"Today I appeal to our President to submit to the will of the people and resign," read the letter published in local media.
"I know that if I were in the President's shoes, I would step down with immediate effect," Kathrada wrote.
In a televised address, Zuma said he would abide by the Constitutional Court's verdict, which ordered him to pay back money spent on a swimming pool, chicken run, cattle enclosure and amphitheatre built at his rural home as so-called "security" measures.
Kathrada, held, like Mandela, as a political prisoner on Robben Island, asked if Zuma was aware that his "outstanding contribution to the liberation struggle stands to be severely tarnished if the remainder of your term as President continues to be dogged by crises, and a growing public loss of confidence in the ANC and government as a whole."
Zuma, 73, whose second presidential term ends in 2019, has also faced scathing criticism over his friendship with the wealthy Gupta family who are said to have undue influence over his government.
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