Deshpande started her career as a teacher at Chhabildas Boy's High School in Dadar, Mumbai, while working here she asked noted playwright, Vijay Tendulkar to write a few plays for her students, this started her association with theatre, and in time made one of the pioneers in experimental theatre movement of the 1960s, as she joined the group Rangayan, which was founded by Vijaya Mehta, Tendulkar, Arvind Deshpande and Shriram Lagoo.
Actors in these theatre groups like Shriram Lagoo, Mohan Agashe, and Sulabha Deshpande brought new authenticity and power to Tendulkar's stories while introducing new sensibilities in Marathi theatre.