The actress, who sang with Marlon Brando in "Guys and Dolls;" costarred with Gregory Peck, Paul Newman and Kirk Douglas; and played Ophelia to Laurence Olivier's Hamlet, died Friday at her home in Santa Monica, her agent Judy Page told the Los Angeles Times. She had lung cancer.
Already a stunning beauty at 14, Simmons made her movie debut in the 1944 British production "Give Us the Moon."
Several minor films followed before British director David Lean gave the London-born actress her breakthrough role of Estella, companion to the reclusive Miss Havisham in 1946's "Great Expectations." That was followed by the exotic "Black Narcissus," and then Olivier's Oscar-winning "Hamlet" in 1948, for which Simmons was nominated as best supporting actress.
She would be nominated for another Oscar, for best actress for 1969's "The Happy Ending," before moving largely to television roles in the 1970s, '80s and '90s.
She won an Emmy Award for her role in the 1980s miniseries "The Thorn Birds."
Her other notable films included "Elmer Gantry" (with Burt Lancaster), "Until They Sail" (with Newman), "The Big Country" (Peck), "Spartacus," (Douglas), "This Earth Is Mine" (Rock Hudson), "All the Way Home" (Robert Preston), "Mister Buddwing" (James Garner) and "Rough Night in Jericho" (Dean Martin).
Simmons had left Britain for Hollywood in 1950, accompanied by her future husband Stewart Granger. There, they were befriended by reclusive tycoon Howard Hughes, who flew them to Tucson, Ariz., for a surprise wedding.
"When I returned from the honeymoon," Simmons told a reporter in 1964, "I learned that Hughes owned me - he had bought me from (British producer) J. Arthur Rank like a piece of meat."
What followed was a string of films that she would later dismiss as terrible, although she took some solace in the fact Hughes, legendary in those days as a womanizer, never bothered her.
"I was married to Jimmy (Granger's real name was James Stewart), so Hughes remained at a distance," she recalled. "But those movies! So terrible they aren't even on videocassettes."
Among the titles: "Angel Face," "Affair with a Stranger" and "She Couldn't Say No."
Simmons finally ended up suing Hughes for the right to make more prestigious films at other studios, and the result was "Young Bess" (as young Queen Elizabeth I), "The Robe" (the first movie filmed in CinemaScope), "The Actress," "The Egyptian" and "Desiree."
In the latter film, in 1954, she played the title role opposite Brando's Napoleon.
The pair teamed again in 1955 for "Guys and Dolls," the Samuel Goldwyn-produced musical in which Simmons is Sarah Brown, a Salvation Army-style reformer conned into a weekend fling in Havana by gambler Sky Masterson.
She loved the rehearsals for that film, Simmons recalled in 1988, "especially the dancing routines with Marlon trying not to step on me and choreographer Michael Kidd looking very worried."
"I got to sing," she added, "because Sam Goldwyn said, `You might as well wreck it with your own voice than somebody else's."'
By the 1970s, her career as a lead film actress had ended, but Simmons continued to work regularly on stage and in television.
In the 1980s and '90s she appeared on such television shows as "Murder, She Wrote," "In the Heat of the Night" and "Xena: Warrior Princess." She also appeared in numerous TV movies and miniseries, including a 1991 version of "Great Expectations," in which she played Miss Havisham this time.
The careers of both Simmons and her husband Granger had flourished in the 1950s, he as a swashbuckler, she as the demure heroine. But long absences on film locations strained their relationship, and they divorced in 1960. They had a daughter, Tracy.
Shortly after her divorce, Simmons married Richard Brooks, who had directed her in "Elmer Gantry" and would again in "The Happy Ending." Their marriage, which produced a daughter, Kate, ended in divorce in 1977.
By Associated Press Writer Bob Thomas