She was born Lelia Vita Goldoni in New York City, of Sicilian ancestry, the daughter of an actor. After her family relocated to California, she spent her upbringing in Los Angeles and eventually attended L.A. City College to study Italian, English literature and psychology. After hours, she performed with the Lester Horton troupe of interpretive dancers. Aged nineteen, she moved back to New York to study drama at a workshop run by John Cassavetes and Burton Lane on West Forty-Sixth Street in Manhattan. Cassavetes gave Goldoni her first break by casting her in his independently produced avant-garde racial drama Gölgeler (1958) as the youngest of three African-American siblings living in a cramped New York apartment. The film focused on their various relationships, on human rather than racial issues. According to Ray Carney in his book 'The Films of John Cassavetes: Pragmatism, Modernism, and the Movies', "Cassavetes was opposed to the notion of art having a negative or satiric agenda, and to works that mocked or denigrated their characters." Carney further asserts that Goldoni "steals most of the scenes in which she appears, not only because her part is so much more emotionally expressive than anyone else's, but because Lelia Goldoni...is brilliantly able to use her face, voice and body to express the smallest flicker of feeling".

Goldoni received the first of her two BAFTA nominations for her role in Shadows. Her unaffected appearance in the picture also set the tone for her future look in subsequent roles. In her own words: "When you do not have regular features you must make the most of your individuality... I like a pale look with the accent on my eyes".

Her next appearance was in an episode of Johnny Staccato (1959), which starred Cassavetes as a jazz piano-playing private detective. Sandwiched in between TV guest spots (and based in Britain for some years) Goldoni headlined as a murderess in the Hammer-produced thriller Hysteria (1965) and then enjoyed a notably animated role pivotal to the gothic drama Ölüm Tiyatrosu (1967), starring opposite horror icon Christopher Lee. Upon her return to the U.S. in 1973, she played Ellen Burstyn's best friend Bea in Alice Artık Burada Oturmuyor (1974) (her second BAFTA nominated performance) and the girlfriend of tough-talking Abe Kusich (Billy Barty) in Çekirgenin Günü (1975), a bitter satire about failed aspirations in 1930s Hollywood. In the remake of Invasion of the Body Snatchers (1978), Goldoni played one of the alien infectees, duplicated as 'a pod person'. She was also a frequent guest star in episodic television, often in crime dramas like Vega$ (1978), Cagney & Lacey (1981), Mike Hammer (1984), Kanun Kanundur (1986) and Cold Case (2003).

A lifelong alumnus of The Actor's Studio, Goldoni later taught acting technique at several institutions, including UCLA and the Lee Strasberg Theatre Institute. As to her own role models, she admitted to being a big fan of actor Stanley Tucci. Goldoni died at the age of 86 at The Actor's Fund Home in Englewood, New Jersey, on July 22 2023.