- Best known for his supporting role as Dr. Heywood Floyd in 2001: A Space Odyssey (1968).
- Although he mostly provided guest starring roles throughout the 1970's upon his return from England to America, he was one of the primary leads of The Gemini Man (created by Steven Bochco) and had a reoccurring part on Quincy, M.E.
- United States lead and second-lead actor who moved to England after World War II, where he trained as an actor. He studied at RADA in 1947 and was the first American member of The Old Vic. He appeared in 1950s and 1960s British pictures and became a fixture on radio and TV, before returning to the United States.
- Seen as wisecracking, virile Americans in low budget British thrillers and horror movies.
- He was going to be the star of the 1956 tv series of The Buccaneers but the part went to Robert Shaw.
- Although he was technically a co-star in 2001: A Space Odyssey, being third billed, his character Dr. Floyd is the main character of the entire segment dealing with the monolith on the moon (the movie's broken up into various parts that are like stories on their own connected as a whole).
- Starred in three movies with Devil in the title: Devil Doll, Devils of Darkness and The Devil Inside.
- Nephew of Raymond Bailey.
- Married twice to actresses, Sylvester was stepfather to his British first wife (Sheila Sweet)'s son for the duration of their marriage. He and his second wife, British actress Veronica Hurst, had three sons.
- While born and raised in America, he trained at RADA and appeared/starred in British television and movies after 1948 until he returned to the USA.
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