Sen was hospitalized in Kolkata more than three weeks ago for treatment of a respiratory infection and died following cardiac arrest, said her daughter, Moon Moon Sen, who is also an actress.
She was to be cremated later Friday.
Sen started acting in 1952 and reigned supreme for 26 years. She won fame in Bengali films, especially co-starring with actor Uttam Kumar. The two become icons for Bengali melodramas and romantic movies through the 1960s and the 1970s. Her most memorable Bengali films included "Agnipariksha," "Devdas" and "Saat Paake Bandha."
The doe-eyed beauty acted in 57 Bengali and seven Hindi films. She shunned public appearances after her retirement from movies in 1978.
Prime Minister Manmohan Singh said Sen had carved a special niche in the hearts of millions of Indians through her graceful cinematic presence. "Her versatility and range of performances mark a unique contribution to Indian cinema, and to Bengali films in particular," he said.
Bollywood superstar Amitabh Bachchan said she "adorned the film world of Bengal with exquisite performances ... She graced Hindi films too!"
"She was a wonder. She was not just a legend," said Mamta Banerjee, West Bengal state's top elected official.
Sen made her debut in Bollywood with the 1955 film "Devdas," co-starring with Dilip Kumar, another legendary actor, and won the best actress award for the movie. Another big Bollywood hit was "Aandhi," in which she played the role of a politician inspired by the life of the then-Indian prime minister, Indira Gandhi.
She was the first Bengali actress to be honored at an international film festival. She was picked best actress at the 1963 Moscow film festival for her role in "Saat Paake Bandha," a Bengali language film. The Indian government honored her with "Padma Shri,'" a top civilian award, in 1972.
She married Dibanath Sen, an industrialist, in 1947 before launching her acting career. Her husband died in the early 1970s.