Her biographer, Peter Villora, said Montiel died at her home in Madrid after passing out. "She was both an actress and singer, but mainly an actress, fulfilling the dream of her life," Villora said.
Montiel was born Maria Antonia Abad in Campo de Criptana in the central region of La Mancha. An acknowledged beauty with an almost husky singing voice, Montiel starred in more than 50 films, many of which were musicals.
She married Anthony Mann, an American actor and film director, in 1957. But press reports, which Montiel never denied, claimed she had turbulent affairs with author Ernest Hemingway and actor James Dean.
She became known for smoking Havana cigars on stage while singing, something that was at the time associated mostly with men. Montiel said it was Hemingway who taught her to smoke.
After limited success in Spain, her career took off in Mexico in the late 1940s where she featured in successful Spanish language films such as "Carcel de Mujeres" (Women's Prison).
From there she made the leap to Hollywood, where she soon attracted the attention of actors and directors. She played a supporting role in the legendary 1955 western "Vera Cruz" alongside actors Gary Cooper and Burt Lancaster.
Her second U.S. film was the musical "Serenade," with tenor Mario Lanza and Joan Fontaine and Vincent Price as stars.
"She was the Spanish star with the greatest international impact until the arrival of Javier (Bardem) and Penelope (Cruz)," Spanish actor Jose Sacristan said.
Having found success in Mexico and the U.S., Montiel then earned star status in her native Spain with 1957's "El Ultimo Cuple" (The Last Couplet), which became one of the highest grossing movies in Spanish cinema history.
The fee for her next film, "La Violetera" (The Violet Seller) netted Montiel more than $1 million, something unheard of for a Spanish star in those days.
In the mid-1970s, Montiel gave up film work and dedicated herself to live musicals on stage and television.
Montiel is survived by her daughter Thais and son Zeus.
Jorge Sainz in Madrid contributed to this obituary.