- He was offered the role of the Second Doctor by Innes Lloyd, the producer of the BBC series Doctor Who (1963), after the departure of William Hartnell but he didn't want to commit himself to a long term role. However, he did appear opposite Patrick Troughton in The Macra Terror: Episode 1 (1967) (which has since been wiped by the BBC) and Tom Baker in The Androids of Tara: Part One (1978).
- He studied at Pembroke College, Cambridge, and performed with the Cambridge Footlights revue society.
- He performed with the Royal Shakespeare Company, the Bristol Old Vic and the National Theatre.
- He attended Harrow public school.
- At the time of Peter Jeffrey's death, some obituaries incorrectly stated that his university was Oxford. It was definitely Cambridge.
- He played Thomas Howard, 3rd Duke of Norfolk, in both Anne of the Thousand Days (1969) and The Prince and the Pauper (1996).
- He achieved the rare distinction of playing a defendant, witness and barrister in different roles in the series Crown Court (1972).
- He acted in both The Avengers (1961) and The New Avengers (1976).
- His speech from If.... (1968) ("Britain today is a powerhouse...") was sampled by pop group Dreadzone on their single "Little Britain". This was released in December 1995, hitting number 20 in the UK.
- He was in the running for the roles of Dr. Armstrong and Sir Percy Heseltine in Lifeforce (1985).
- He played Sherlock Holmes in The Best House in London (1969) and his elder brother Mycroft in Hands of a Murderer (1990).
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