Harrold was born in Tazewell, Virginia, to B.H. and Carolyn Harrold. She attended Tazewell High School and Mills College in Oakland, California, majoring in drama. She studied acting at HB Studio in New York City.
Harrold was Steve McQueen's leading lady in the screen legend's final film, The Hunter (1980), and Arnold Schwarzenegger's leading lady in the action vehicle Raw Deal (1986). She appeared in Nightwing (1979), The Pursuit of D. B. Cooper (1981), the cult horror film The Sender (1982), and co-starred with Luciano Pavarotti in Yes, Giorgio (1982). Harrold starred in Modern Romance (1981) as the ex-girlfriend of Albert Brooks's character. Harrold also had a supporting role in Into the Night (1985), an action/suspense film directed by John Landis, as Paul Mazursky's character's girlfriend.
Harrold began her television career playing Nola Dancy Aldrich on the NBC daytime soap opera The Doctors from 1976 to 1977. After she left the show, her replacement was Kathleen Turner. In 1978-9 she appeared in several episodes of The Rockford Files, as a blind psychiatrist with whom Rockford was in love. In the 1980s, she had the leading roles in the short-lived dramas MacGruder and Loud (1985), produced by Aaron Spelling, and The Bronx Zoo (1987–88), opposite Ed Asner. From 1991 to 1993, she co-starred alongside Regina Taylor and Sam Waterston in the NBC period drama I'll Fly Away. She later was a regular cast member on The Larry Sanders Show, playing Francine Sanders.

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