Moore's family confirmed the news by posting a statement on the actor's official Twitter page.
"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 love with which he was surrounded in his final days was so great it cannot be quantified in words alone," read the statement signed by Moore's children, Deborah, Geoffrey and Christian.
With seven Bond films, Moore played the role more often than any of the other Bonds such as Sean Connery and Daniel Craig. He acted in films such as Live and Let Die" and "The Spy Who Loved Me".
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In their statement, the family said Moore considered his work for UNICEF as his "greatest achievement".
"The affection our father felt whenever he walked onto a stage or in front of a camera buoyed him hugely and kept him busy working into his 90th year... In accordance with our father's wishes there will be a private funeral in Monaco."
Besides his outings as Bond, Moore had an extensive and productive career as an actor in cinema and television.
His other prominent performance were in films such as "Bullseye!", "Bed & Breakfast", "Curse of the Pink Panther" and "The Quest".
On small screen, Moore was popular for doing "Ivanhoe", "The Saint" and "The Persuaders".
Moore penned two books about his time as Bond as well as two autobiographies, including "My Word is My Bond: The Autobiography", which was peppered with anecdotes about his encounters with other stars and his memories of his time in Hollywood.
Celebrities across the globe expressed their grief over Moore's demise.
"Roger Moore , loved him," Oscar-winning actor Russell Crowe tweeted.
Kris Jenner posted, "The ultimate James Bond... So sad to hear that Roger Moore has passed away. Thoughts and prayers are with his family..."
Actress Mia Farrow wrote, "Few are as kind and giving as was Roger Moore. Loving thoughts with his family and friends. He will be missed too by UNICEF."
Bollywood actors Rishi Kapoor and Boman Irani also mourned Moore's demise.
"RIP. Name is James... Roger Moore... Bond," Kapoor wrote alongside Moore's picture.