Patekar was rushed to a hospital after he fell unconscious at his flat in the early hours of Thursday.
‘Despite 45 minutes of continuous CPR, he could not be revived,’ Dr Shekhar Salkar of Manipal Hospital in Goa told a news agency.
Patekar appeared in dozens of successful Bollywood films and was also a prominent figure in theatre and regional cinema, particularly Marathi-language productions.
He made his film debut in Gaman in 1978 and went on to play supporting roles in several films. His intense screen presence, however, soon brought him wider recognition.
His breakthrough came with Parinda in 1989, in which he played the volatile gangster Anna. The performance earned him his first National Film Award and Filmfare Award and established him as a major actor in Indian cinema.
Patekar went on to deliver a series of memorable performances during the 1990s, demonstrating his versatility across a wide range of characters.
He received acclaim for his portrayal of Major Chauhan in Prahaar, a film he also directed. He also played Majid Khan in Angaar, the patriotic firebrand in Tirangaa, and Pratap Narayan Tilak in Krantiveer.
His performance in Krantiveer earned him the National Film Award for Best Actor.
Just when critics thought that playing loud characters was his mainstay, he proved them wrong by delivering a mesmerising performance in Khamoshi as a person who could not hear or speak.
Patekar was also known for his activism and didn't mince his words while criticising the government of the day.
Issues related to farmers were particularly close to his heart.
Financial Mirror/AH