- Was so fond of the role of The Master that, according to Doctor Who script editor Eric Saward, Ainley would introduce himself on the phone by saying "This is the Master," and then do his trademark villainous laugh.
- Just as his Doctor Who character "The Master" would use anagrams to conceal his identity, Ainley would be credited with an anagram of his own name to hide the fact that a character he was playing in certain episodes was The Master in Disguise. Most notably, this led to his credit in "Castrovalva" episode 3 being "Neil Toynay" (Tony Ainley).
- He would often turn down acting roles that would clash with major cricket matches.
- He played the Master in 'Doctor Who' for nine years - the longest serving actor to appear as a regular character in the TV series' history.
- He despised cheeses of all kinds.
- After Roger Delgado, Peter Pratt and Geoffrey Beevers, he was the fourth actor to play the Master, the Doctor's greatest enemy, in Doctor Who (1963). He played the role from the 1981 serial "The Keeper of Traken" to the 1989 serial "Survival". He is the longest running Master. He was succeeded in the role by Gordon Tipple, Eric Roberts, Sir Derek Jacobi and John Simm.
- Before his acting career took off, he was well known as a leading rugby player in London, playing under the name of A.A. Holmes. For several seasons in the sixties he played regularly for Richmond and Middlesex, either at full back or centre three quarter. Articles confirming this can be found in the archives of the London Evening Standard, written by the then rugby correspondent Richard Evans. Photographs accompanying the articles clearly confirm that Holmes and Ainley are one and the same.
- Was a keen club cricketer - even abruptly citing Sophie Aldred (who played Ace on Doctor Who) as his friend once he learned that she played cricket.
- By the mid-eighties, he had come into some money that allowed him to live a comfortable life without acting. He actually rejected many TV and film roles in 80s and 90s because of this.
- He was on the shortlist for Prof. Watson (played by Glyn Houston) in Doctor Who: The Hand of Fear.
- He was a keen cricketer for many years.
- Succeeded, briefly, in the role of the Master by Gordon Tipple, and then, more fully, by Eric Roberts, who portrayed the villain in Doctor Who: The Movie (1996).
- Considered for Dr. Armstrong, Sir Percy Heseltine and Dr. Bukovsky in Lifeforce (1985). He was offered a role in the film but turned it down.
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