Doyle was born in Omaha, Nebraska, the son of Mary Ruth (née Fitzgerald) and Lewis Raymond Doyle, an attorney. His maternal grandfather, John Fitzgerald, was a prominent railroad builder and banker in Nebraska. He graduated from Campion High School in Prairie du Chien, Wisconsin, in 1947.
He is best remembered for his role as detective John Bosley on the television series Charlie's Angels, appearing in all 110 episodes of the series (1976-81) along with original cast member Jaclyn Smith and an all-girl cast. He also lent his distinctive raspy voice to the character Grandpa Lou Pickels in the Nickelodeon animated series Rugrats until his death in 1977. Since then, Joe Alaskey assumed the role of Grandpa Lou. Doyle made a number of appearances as a guest on the game show Match Game in the late 1970s and early 1980s, more often than not giving bizarre answers that seldom matched the contestants. He usually sat in the top row next to Brett Somers and Charles Nelson Reilly. He appeared on one week of Password Plus in 1980, three weeks of Super Password, and appeared on Tattletales with his wife Anne in 1982.
Doyle was a reputable stage actor as well. He played Orgon in the 1964 premier of Richard Wilbur's translation of Tartuffe at the Fred Miller Theater in Milwaukee. His sister, Mary Mulry Doyle, played the fulminate maid, Dorisse. Steven Porter directed the production.
- TaleSpin - Sheriff Gomer Cleghorn
- Darkwing Duck - Adopt-A-con Judge
- Bonkers - W.W. Wacky
- Quack Pack - Father Roborson
- Mighty Ducks - Sam Delaney
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