After playing roles in many dramas including Shakespeare, he became known for portraying the title role of the children's series Catweazle (1970–72), after turning down the opportunity to play both the First and Second Doctors in the long-running BBC science fiction television series Doctor Who. Bayldon's other long-running parts include the Crowman in Worzel Gummidge (1979–81) and Magic Grandad in the BBC television series Watch (1995).
Bayldon made several film appearances in the 1960s and 1970s, including King Rat (1965), To Sir, with Love (1967), Casino Royale (1967), the Envy segment of The Magnificent Seven Deadly Sins (1971), the Marc Bolan/T. Rex film Born To Boogie and the film version (Porridge) of the television series Porridge (1979) as the Governor.
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