Carr was born Charmian Farnon in Chicago, Illinois, the second child of vaudeville actress Rita Oehman and musician Brian Farnon. She has two sisters, both actresses (Shannon Farnon and Darleen Carr).
While Charmian was attending college part-time and working for a doctor, her mother arranged for her to audition for a role in The Sound of Music. Rita Farnon hadn't asked Charmian if she wanted to audition for the part, but Charmian was sure her mother would consider getting a part in a film more important than earning a college diploma. Director Robert Wise thought Farnon was too long a surname. After he had given her a list of single syllable surnames, she chose Carr. She won the role of Liesl over Geraldine Chaplin, Patty Duke, Mia Farrow and Sharon Tate.
The film was on the whole a very happy experience for her. However, during the filming of her dance scene with Rolf in the gazebo, the costumers had forgotten to put no-slip pads on her shoes, she slid through a window of the gazebo, and she "had to complete the scene in agony".
She owns and operates an interior design firm, Charmian Carr Designs, in Encino, California. Her clients included Ernest Lehman, screenwriter for The Sound of Music; Michael Jackson, who hired her because he was a fan of the film; and other cast members from the film. On December 12, 2007, Carr made a rare television appearance as a guest on Loose Women, wherein she shared some of her memories of making The Sound of Music with the hosts.
She has written two books, Forever Liesl and Letters to Liesl.
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While publicizing The Sound of Music after its release, Carr met Jay A. Brent, whom she married on May 21, 1967. She retired from acting to raise her two daughters, Jennifer and Emily, and to establish an interior design company. The marriage was dissolved in 1991; Carr has not remarried.