The actress was suffering from ovarian cancer and had been in the Jaslok hospital for last couple of months. She died at around 2.30 AM today, a top official of the hospital said.
Talwalkar, who had an advanced-stage cancer, yesterday complained of breathlessness. The doctors tried to revive her, but in vain, the official said.
The cremation will be held later today.
Prime Minister Narendra Modi has expressed grief over the passing away of veteran film personality. Modi said her demise is a major loss to Marathi film industry. He even recalled Smita's contribution to the Marathi film industry and prayed that her soul rests in peace.
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The National-award winning actress acted in films like 'Tu Saubhagyavati Ho' and 'Gadbad Ghotala', where she featured along with noted actors Laxmikant Berde, Ashok Saraf and Nilu Phule.
Information and Broadcasting minister Prakash Javadekar also took to Twitter to express his grief.
"Legendary actress, director, producer Smita Talwalkar ll remain in hearts of people. May her soul #RIP. My condolences to the bereaved," he tweeted.
Talwalkar turned film producer with 'Kalat Nakalat' under the banner 'Asmita Chitra' in 1989. The film won a National Film Awards in 1991.