Anand's good looks and skill as a leading man earned him the nickname "Adonis of India" and landed him acting and producing roles in dozens of Indian films, the BBC said Sunday.
"An era has come to an end. Dev Anand leaves a void never perhaps to be filled again. He never gave up belief, his joy of life," Bollywood superstar Amitabh Bachchan said in a Twitter tweet after hearing the news.
Family members said Anand had not been feeling well and was in London for a checkup.
Anand's 65-year career in the industry kept busy until the end. He directed "Chargesheet," which was released in September.
IBN Live said Anand was the undisputed top star of Bollywood's black-and-white area and the news of his death rippled across India.
President Pratibha Patil, Prime Minister Manmohan Singh and Speaker Meira Kumar were among the national leaders who issued written statements of condolence. "Dev Anand was a great artiste who entertained generations of cinema lovers over five decades," said Singh. "He was an embodiment of a life-long passion for acting and film making."