Peters, 75, played Pat, a nurse tending to Sean Connery's Bond in 1965's "Thunderball." She was the first Bond girl to take her clothes off onscreen in scenes that were considered racy and controversial at the time. Several were ultimately cut from the film.
The Bond Twitter feed said: "We are sad to hear that Molly Peters has passed away at the age of 75. Our thoughts are with her family."
Peters' death comes barely a week after that of Roger Moore, who played the part of the suave 007 more times than any other actor.
See photos of Molly Peters:
Molly Peters through the years
Molly Peters through the years
Molly Peters with a white sheet wrapped around her and holding it up with her left arm across her chest in a scene from the film 'Thunderball', 1965. (Photo by United Artists/Getty Images)
Scottish actor Sean Connery and American actress Molly Peters on the set of Thunderball. (Photo by Sunset Boulevard/Corbis via Getty Images)
Molly Peters getting her back rubbed by Sean Connery who is wearing a robe in a scene from the film 'Thunderball', 1965. (Photo by United Artists/Getty Images)
Portrait of actress Molly Peters, former Bond girl in the film 'Thunderball', standing in a London park prior to her appearance in the West End, England, circa 1965. (Photo by Keystone Features/Hulton Archive/Getty Images)
Actor Sean Connery with (left to right), Lois Maxwell, Luciana Paluzzi, Martine Beswick, Claudine Auger and Molly Peters, his female co-stars from the film 'Thunderball', 1965. (Photo by United Artists/Getty Images)
Molly Peters rubs Sean Connery back with a fur mitten in a scene from the film 'Thunderball', 1965. (Photo by United Artists/Getty Images)
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Peters, who was also a model, had a fleeting acting career, spanning just a handful of films and series in the mid-1960s. "Thunderball" was her most notable big screen role.
Her movie career ended with the 1968 feature "Don't Raise the Bridge, Lower the River." She also had parts in various 1960s series, including "Armchair Theater."
In later life, she talked about her Bond role in 1995's "Behind the Scenes With Thunderball" and 2000's "Terence Young: Bond Vivant."
The cause of death has not been announced.
We are sad to hear that Molly Peters has passed away at the age of 75. Our thoughts are with her family. pic.twitter.com/6k3Ifs2gpY
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