Suchitra Sen had been admitted to a hospital in Calcutta last month with a chest infection and her condition worsened on Thursday night, doctors said.
Known as the Greta Garbo of India for leading a reclusive life after she left films, Suchitra Sen was an iconic star of regional Bengali cinema.
She also acted in a number of Bollywood films such as Devdas and Aandhi.
Suchitra Sen teamed up with Bengali star Uttam Kumar to form a popular pair that delivered a series of hits in Bengali cinema for over two decades.
She quit films in 1978 and led a hermit-like existence, reportedly refusing to meet people outside her own family. She had not been seen in public or photographed in the past three decades.
Suchitra Sen made her debut in 1953 with the hugely popular comedy Share Chuattar (Seventy-four-and-a-half), which was also her first film with Kumar.
Her performance as a nurse hired by a psychiatrist to develop personal relationships with male patients in the 1959 film Deep Jwele Jaai was hailed as one of her best.
Suchitra Sen is survived by her actress daughter Moon Moon Sen. Her grand daughters, Riya and Raima Sen, are also actresses.
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