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Cynthia began her career in 1968 by casting penises of rock musicians. She later expanded her subjects to include filmmakers and other types of artists. By 2000 she had begun casting female artists' breasts.
Shy as a young girl, Cynthia sought out a way to make contact with the opposite sex. In the late-1960s she became caught up in free love and rock music. In college, when her art teacher gave the class an assignment to, "plaster cast something solid that could retain its shape", her idea to use the assignment as a lure to entice rock stars to have sex with her became a hit, even before she made a cast of anyone's genitalia. Finding a dental moldmaking substance called alginate to be sufficient, she found her first client in Jimi Hendrix, the first of many to submit to the idea.
Meeting Frank Zappa, who found the concept of "casting" both humorous and creative as an art form, though he himself never submitted to the procedure, Albritton found in him something of a patron. He moved her to Los Angeles, California, which she described as a veritable groupie heaven, with no lack of assistants. Together, Zappa and Albritton conceived an idea of preserving the casts of musicians for a future exhibition, entrusting them to his partner, Herb Cohen, for safekeeping. This idea never took off, due to a lack of famous rock stars as participants. A movie was made of Cynthia Plaster Caster, and her celebrity grew. However, she found herself having to file a lawsuit to retrieve the casts.  She decided to cast women's breasts as well in 2000.
A film documentary, Plaster Caster (2001), has been made about her, she has inspired at least two songs: "Five Short Minutes" by Jim Croce. and "Plaster Caster" by Kiss and she is also mentioned in the Le Tigre song "Nanny Nanny Boo Boo".