One of the most recognisable faces of Indian cinema, Patekar won three National Film Awards and became known for playing complex, often volatile characters. He was also a prominent figure in Marathi language cinema and theatre.
He was rushed to hospital after being found unconscious at his home in Goa 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 ANI news agency.
On Thursday, Prime Minister Narendra Modi led tributes to the actor, praising Patekar's versatility and outspoken personality.
Patekar portrayed characters that would "remain etched in the memory of generations", Modi wrote on X, adding that his death had left "a vast void in the artistic world".
Bollywood star Akshay Kumar, who appeared alongside Patekar in the comedy film Welcome, remembered him as a rare performer whose voice, intensity and honesty could command an audience's attention.
Patekar made his debut with the film Gaman in 1978 and continued to play smaller roles in several films. But the intensity that he brought on the screen was hard to miss and soon he landed a role in Parinda in 1989, making him a household name across India. He won his first National Film Award and the Filmfare Award as well for his portrayal of the gangster Anna in the film.