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Loren became an international film star with a five-picture contract with Paramount Studios. Among her films at this time: Desire Under the Elms with Anthony Perkins, based upon the Eugene O'Neill play; Houseboat, a romantic comedy co-starring Cary Grant; and George Cukor's Heller in Pink Tights in which she appeared with blond hair (a wig) for the first time. Loren demonstrated considerable dramatic skills and attracted respect as a dramatic and comedic actress, especially in Italian projects where she could express herself more freely, although she acquired great proficiency in English.

In 1960, her acclaimed performance in Vittorio De Sica's Two Women earned many awards, including the Cannes, Venice and Berlin Film Festivals' best performance prizes. Her performance was also awarded an Academy Award for Best Actress, the first major Academy Award for a non-English-language performance. Initially, the stark, gritty story of a mother and daughter surviving in war-torn Italy was to cast Anna Magnani as Sophia's mother. Negotiations, perhaps due to billing, broke down and the screenplay was rewritten to make Sophia the mother; Eleonora Brown portrayed the daughter.

Belying the typical portrayal of the beautiful actress as vacuous and emptyheaded, Loren was known for her sharp wit and insight. One of her most frequently-quoted sayings is her quip about her famously-voluptuous figure: "Everything you see, I owe to spaghetti."

During the 1960s Loren was one of the most popular actresses in the world, and she continued to make films in both the U.S. and Europe, acting with leading male stars. In 1964, her career reached its zenith when she received $1 million to act in The Fall of the Roman Empire.

Among her best-known films of this period are The Millionairess (1960) with Peter Sellers, Vittorio De Sica’s triptych Ieri, oggi, domani (1963) with Marcello Mastroianni, Peter Ustinov's Lady L (1965) with Paul Newman, and Charlie Chaplin's final film, A Countess from Hong Kong (1967) with Marlon Brando.

Despite the failure of many of her films to generate sales at the box office, she has an impressive roster of credits and work with famous co-stars. Invariably, she has turned in a charming performance and worn some of the most lavish costumes ever created for the movies. Some of her most attractive performances include A Breath of Scandal (1960), Madame Sans-Gêne (1962), Heller in Pink Tights (1960) and More Than A Miracle (1967).

Loren also recorded well over two dozen songs throughout her career, including a best-selling album of comedic songs with Peter Sellers; reportedly, she had to fend off his romantic advances. It was partly due to Sellers' infatuation with Loren that he split with his first wife, Anne Howe. Loren has made it clear to numerous biographers that Seller's affections were reciprocated only platonically. This collaboration was covered in The Life and Death of Peter Sellers where actress Sonia Aquino portrayed Loren.

Her struggle to have children was of worldwide interest. Having suffered two very physically and emotionally-painful miscarriages, she was referred to Swiss fertility specialist Dr. Huebert de Watteville. He determined that Loren was deficient in estrogen, and after he prescribed regular injections of the hormone and bed rest for her entire term, Loren became a mother twice. She has proudly stated that the births of her sons meant more to her than anything else she had accomplished in her life.

Once she achieved motherhood, Loren worked less. She moved into her 40's and 50's with roles in films including the last De Sica movie, The Voyage, with Richard Burton and Ettore Scola's A Special Day with Mastroianni.

In 1980, she portrayed herself, as well as her mother, in a made-for-television biopic adaptation of her autobiography. Actresses, Ritza Brown and Chiara Ferrari played Loren at younger ages. She made headlines in 1982 when she served an 18-day prison sentence in Italy on tax evasion charges, a fact that didn't damage her career or popularity.

In her 60s, Loren became selective about choosing her films and ventured into various areas of business, including cook books, eyewear, jewelry and perfume. She also made well-received appearances in Robert Altman's Ready to Wear and the 1995 comedy Grumpier Old Men playing a femme fatale opposite Walter Matthau and Jack Lemmon.

In 1991, Loren received an honorary Academy Award for her contribution to world cinema and was declared "one of the world cinema's treasures".