- Descendant of the Earls of Clarendon.
- Had a long-standing friendship with fellow actors Peter O'Toole and Peter Bowles.
- One of James's best friends was actor Ronald Fraser. They worked together in the 1973 TV version of Pygmalion. Nicholas Whittaker, author of Platform Souls And Blue Period, worked in the Belsize Tavern in 1979 and 1980 and recalls Villiers' visits to the pub in the company of Fraser. After closing time, the pair would often be found in the Beer & Curry Restaurant opposite.
- In The First Churchills (1969), he played King Charles II of England, the lover of his distant relative Barbara Palmer, 1st Duchess of Cleveland.
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