Paul Zimet was born and raised in New York City, where he attended the High School of Music and Art. He studied comparative literature at Columbia University and medicine at Harvard Medical School. After producing plays at the medical school and Harvard College, he decided to pursue theatre full-time. He directed plays at Judson Poets Theater and other venues in New York City and taught elementary school science. In 1967, he joined Joseph Chaikin's Open Theater, where he performed in AMERICA HURRAH (1966), THE SERPENT (1970), TERMINAL (1970), THE MUTATION SHOW (1973), and NIGHTWALK (1973). He received three OBIE awards while with The Open Theater and The Winter Project.

Zimet then went on to found The Talking Band theatre company with some other former members of the Open Theater. He received an OBIE award for his direction of PAINTED SNAKE IN A PAINTED CHAIR (2003). Other productions of note include: HOT LUNCH APOSTLES (1983), BETTY AND THE BLENDERS (1987), and THE GOLDEN TOAD (2015). Zimet has taught at Princeton, Williams, NYU, and Fordham and is Associate Professor Emeritus in Theatre at Smith College. He is an alumnus of New Dramatists.