The iconic actor died after a battle with acute leukaemia, his manager, Matthew Sullivan, confirmed to Deadline.
"Mr Vaughn passed away with his family around him in New York," Sullivan said.
Vaughn's lengthy list of credits include "Magnificent Seven", "Bullitt", "Towering Inferno" and television roles in "Hustle" and "Coronation Street". But, he will no doubt be remembered for Napoleon Solo.
UNCLE aired from 1964-68, and paired Vaughn's elegant, dark-haired Solo with David McCallum's blond Russian Illya Kuryakin.
The actor earned a supporting Emmy for the 1977 "Washington: Behind Closed Doors" and an Emmy nomination for playing Woodrow Wilson in "Backstairs at the White House" (1979).
Vaughn also appeared onstage, including a 1955 production of The Pilgramage Play in Hollywood, later taking roles in Tom Stoppard's "The Real Inspector Hound" and more recently, "Twelve Angry Men" at the Birmingham Repertory Theatre in 2013.
He is survived by his wife Linda and two children, Cassidy and Caitlin Vaughn.
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