He died peacefully in his sleep surrounded by wife Micheline and his two sons, Jason and Stephane, his publicist told the British Press Association.
Handpicked by creator Ian Fleming, Connery embodied "Bond, James Bond" for millions as the suave drinker, womanizer and disposer of evil.
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He starred in seven films as Agent 007: "Dr. No" (1962) "From Russia with Love" (1963), "Goldfinger" (1964), "Thunderball" (1965), and "You Only Live Twice" (1967) -- then appeared again in "Diamonds Are Forever" (1971) and "Never Say Never Again" (1983).
"We are devastated by the news of the passing of Sir Sean Connery. He was and shall always be remembered as the original James Bond ... he revolutionised the world with his gritty and witty portrayal of the sexy and charismatic secret agent. He is undoubtedly largely responsible for the success of the film series and we shall be forever grateful to him," James Bond franchise producers Barbara Broccoli and Michael G. Wilson said in a statement.
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Thirty years into his film career, Connery won his first Oscar in 1988 for his portrayal of the steely Irish cop in "The Untouchables." "Patience is truly a virtue," he told the audience during a standing ovation.
He also had major roles in films including "Indiana Jones and the Last Crusade," "Highlander" and "The Hunt for Red October."
At the turn of the new millennium, the actor was named "Sexiest Man of the Century by New Woman magazine and the Web site Women.com. He was knighted by Queen Elizabeth II in 2000 for services to film drama.
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The Associated Press contributed to this report.