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Hurst was born in the Villa Palmera neighborhood of San Juan, Puerto Rico, a middle-class area. Her father owned the "Farmacia Imperial" (Imperial Pharmacy) in Barrio Obrero. She is also a cousin of Puerto Rican TV producer Tommy Muñiz. Hurst completed her primary and secondary schooling in San Juan.
From a young age, Hurst expressed her desire to become an actress to her parents, who then enrolled her in Ana Santisteban's modeling academy. In 1960, at age 17, while joking around with friends waiting at the academy, producer Gaspar Pumarejo spotted her as he searched for fresh talent for a new show.
That same year, Hurst was hired to star in the TV comedy Pompilia y su Familia (Pompilia and her Family), aired on WAPA-TV. She later hosted La Hora del Niño (The Children's Hour) on Channel 6. During the 1960s, she appeared in other comedies such as Casos y Cosas de la Casa (Cases and Things of the House) alongside Braulio Castillo, and Matrimonio y Algo Más (Marriage and Something More). In 1969, she worked for a year on the Peruvian program El Hit del Momento (The Hit of the Moment) with Panamericana de Television in Lima.
Upon returning to Puerto Rico, Hurst participated in several shows produced by her cousin Tommy Muñiz and began acting in theater. Her stage credits include La Casa de las Hojas Azules (The House with the Blue Leaves) and La Verdadera Historia de Pedro Navaja (The True Story of Pedro Navaja). In 1980, she wrote and produced a stage show performed at the Condado Beach Hotel in San Juan.
Hurst then moved to New York, where she briefly worked in Off-Broadway productions. In 1989, she relocated to Los Angeles, California, enrolled at Santa Monica College, and majored in psychology. She acted in both Spanish and English productions, including the role of Mrs. Maris in Windows (1991) at the Taper Forum Theater and Lola in La Balada de Tina Jaurez (The Ballad of Tina Juarez) (1992). Additionally, she founded an acting school for Hispanic children.
Hurst has appeared in twenty films, including the 2005 release English as a Second Language. She has also guest-starred in over thirty television episodes on shows such as JAG, NYPD Blue, The X-Files, ER, Lost, and had a recurring role as Celia in sixteen episodes of Dharma and Greg. She portrayed Yolanda Salazar, Betty Suarez's grandmother, in the Ugly Betty episode "A Tree Grows in Guadalajara." As of 2007, Lillian Hurst was living in Los Angeles, continuing her acting career.
