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Keays-Byrne was born in Srinagar, in the state of Jammu and Kashmir (part of the British Raj then, India now) to British parents; his family returned to Britain when India was partitioned. He began his career as a stage actor.

Keays-Byrne made his first television appearance in 1967 on the British television programme Boy Meets Girl. He was part of Peter Brook's production of A Midsummer Night's Dream with the Royal Shakespeare Company, which toured Australia in 1973. Keays-Byrne decided to remain in Australia after the tour ended. In 1974, he acted in the TV movie Essington, then made his first film appearance in the motorcycle picture Stone (1974). This was followed by supporting roles in films like The Man from Hong Kong (1975), Mad Dog Morgan (1976), The Trespassers (1976) and Snapshot (1979).

After his first starring role in the 1978 TV movie Death Train, Keays-Byrne was cast as the violent gang leader Toecutter in Mad Max (1979). Director George Miller had Keays-Byrne and the other actors for the gang travel from Sydney to Melbourne in a group on motorcycles, as there was no money for airplane tickets. In an early international print of the film, Keays-Byrne was dubbed with a bad American accent, which Miller later regretted.

Keays-Byrne then continued to act in post-apocalyptic and science fiction films like The Chain Reaction (1980), Strikebound (1984), Starship (1985) and The Blood of Heroes (1989). In 1992, he made his directorial debut and acted in the film Resistance. He also appeared in TV miniseries adaptations of Moby Dick (1998) and Journey to the Centre of the Earth (1999).

Keays-Byrne played Grunchlk in the science fiction television series Farscape (1999–2003) and its conclusion Farscape: The Peacekeeper Wars (2004). George Miller also cast him as the Martian Manhunter in the planned 2009 movie Justice League: Mortal.

Keays-Byrne returned to the Mad Max franchise in the 2015 film Mad Max: Fury Road as the main villain Immortan Joe. The film was nominated for 10 Academy Awards, including Best Picture, winning 6, and Keays-Byrne was nominated for the MTV Movie Award for Best Villain.