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The star of movies such as "City of Joy" and "East Is East" suffered a heart attack early Friday at his Mumbai home, according to a close friend.
"He was a torchbearer of Indian cinema," actor Anupam Kher told CNN, describing Puri as "a wonderful friend and an amazing person."
Puri was known for his versatility and appeal across global markets. He appeared not only in mainstream Bollywood movies and regional Indian cinema but also British and Hollywood productions.
Puri was one of the lead stars of 2014's "The Hundred-Foot Journey" and also appeared in 2007's "Charlie Wilson's War" and 2012's "The Reluctant Fundamentalist."
Breaking the mold
"In the 1970s and '80s, there was a certain chocolatey look required to be a part of Indian cinema. Om Puri broke that myth with sheer talent and hard work," Kher said.
Puri trained at India's National School of Drama and the Film and the Television Institute of India.
"He had humble beginnings," Kher said, "but the glamour of Bollywood didn't affect him."
"He didn't let himself change."
Puri won numerous awards for his work. In 1990, he was honored with the Padma Shri, India's fourth highest civilian honor, for his contribution to the arts.
In 2004, he was awarded an honorary Order of the British Empire for his contributions to the UK film industry. Puri also received best actor honors twice at India's National Film Awards.
Hits such as "Ardh Satya" and the satirical "Jaane Bhi Do Yaaron" -- both from 1983 -- led to widespread recognition for Puri in his home country.
A number of top Indian leaders, actors, and sports stars posted tributes to the actor on social media Friday.
Indian Prime Minister Narendra Modi offered condolences, as did many members of Bollywood's film community.
Cricketer Sachin Tendulkar said, "You will live in our hearts forever."