- Appeared as a butler in the rock and roll movie Born to Boogie (1972) featuring Marc Bolan and T. Rex, and directed by Ringo Starr, due to their fondness for his TV series Catweazle (1970).
- At the age of 80 in 2004, he became the oldest actor to ever play the Doctor Who (1963) character the Doctor, which he did (for the second time) in the Big Finish audio drama "A Storm of Angels".
- He played the Doctor in two "Doctor Who Unbound" audio plays, "Auld Mortality" (2003) and "A Storm Of Angels" (2005).
- He served in the Royal Air Force prior to training to be an actor.
- Trained as an RAF air-crew radio operator during the war but by the time his training was complete there were sufficient crews so he worked in orderly rooms and helped with entertainment.
- He was the long-term partner of fellow actor Alan Rowe, who died in 2000.
- Has said in an interview he was offered the role of the first Doctor Who (played by William Hartnell). This is at odds with most documents of the official history of the series, which have stated that Hartnell was the third choice after Cyril Cusack and Leslie French. Bayldon was considered for several roles in the series, including Sir Robert Muir in Black Orchid: Part One (1982), Lord President Borusa in Arc of Infinity: Part One (1983)and Lord Ravensworth in The Mark of the Rani: Part One (1985).
- He was considered for the roles of Dr. Hans Fallada, Dr. Armstrong, Sir Percy Heseltine and the Fatherly Guard in Lifeforce (1985).
- He died only seven days after his Casino Royale (1967) co-star Daliah Lavi.
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