He was born in Soweto. After having to give up his studies owing to poverty, after 1946 he experienced worker exploitation as a factory worker. When working as a bus driver, he was active in a strike for better working conditions and a living wage, and in 1951 joined the African National Congress Youth League (ANCYL) and, in 1954, the African National Congress (ANC).

In 1961, he was sent for military training outside the country, but on his return in 1963 was arrested, after being accused of recruiting and training an armed force. He was found guilty and sentenced to life imprisonment on Robben Island.

He was married to June Mlangeni and they have five children, his wife died in 2001.

After his release from prison 27 years later, Mlangeni served as a member of parliament for the ANC from 1994 to 1999. He served once more in the National Assembly from 2009 until 2014, when he retired.

He was close friends with Nelson Mandela and spoke at Mandela's memorial service at FNB Stadium.

In 2015, director Lebogang Rasethaba made a film about Mlangeni, entitled Prisoner 467/64: The Untold Legacy of Andrew Mlangeni.

In 2017, Mlangeni appeared with fellow defendants at the Rivonia Trial, Denis Goldberg and Ahmed Kathrada, along with lawyers Joel Joffe, George Bizos and Denis Kuny in a documentary film entitled "Life is Wonderful", directed by Sir Nicholas Stadlen, which tells the story of the trial. (The title reflects Goldberg's words to his mother at the end of the trial on hearing that he and his comrades had been spared the death sentence).

On 26 April 2018, Mlangeni received an Honorary Doctorate in Education from the Durban University of Technology in South Africa. He was also awarded an Honorary Doctorate in Law on 7 April, 2018 by Rhodes University.

Mlangeni was awarded the Freedom of the City of London on 20 July 2018. On that visit, he was also a guest of honour at the opening of the Mandela Centenary Exhibition at the South Bank Centre, alongside Their Royal Highnesses, the Duke and Duchess of Sussex. On the Centenary Celebration of Nelson Mandela's birth, he also read Mandela's favourite poem - Invictus - which was aired on the BBC's Newsnight programme.

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