The veteran actor died in Switzerland after a short battle with cancer, according to a message from his family shared on the actor's official Twitter account.
"With the heaviest of hearts, we must share the awful news that our father, Sir Roger Moore, passed away today. We are all devastated," the message read.
MORE: Roger Moore through the years
Sire Roger Moore through the years
Moore starred in seven James Bond movies in the 1970s and 1980s, including "Live and Let Die," "The Man With the Golden Gun," "The Spy Who Loved Me," "Octopussy," "Moonraker," "For Your Eyes Only" and "A View to a Kill."
He kept acting until recently, appearing in a stage production in London last November.
Roger Moore, famed James Bond actor, dies at 89
His children said in addition to acting, Moore was dedicated to his work with the relief organization UNICEF.
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Moore received the Dag Hammarskjold Inspiration Award for his work with UNICEF and was named a commander in France's National Order of Arts and Letters in 2008, an award he said was worth "more than an Oscar."
That same year he published an autobiography, "My Word Is My Bond," which included details about his work on the Bond films, his friendship with Audrey Hepburn, his encounters with Cary Grant, Frank Sinatra, Elizabeth Taylor and other stars, and his health struggles - including a bout with prostate cancer, which he beat.
Moore was divorced three times, from skater Doorn Van Steyn in 1953, English singer Dorothy Squires in 1969 and Italian actress Luisa Mattioli, the mother of his children Deborah, Geoffrey and Christian, in 2000.
He married a fourth time, in 2002, to Swedish socialite Kristina Tholstrup.
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The Associated Press contributed to this report.