Ajit Wadekar, the man who led India to their first series triumphs in England and the West Indies, died on Wednesday at the age of 77, the Press Trust of India reported.
Wadekar died at a hospital in Mumbai after battling a prolonged illness, the news agency said.
The former batsman, who led India to victories in England and the West Indies in 1971, scored 2,113 runs in just 37 Test matches, including one century.
Tributes poured in on social media for Wadekar, with Indian Prime Minister Narendra Modi hailing him as "a great batsman & wonderful captain".
"He led our team to some of the most memorable victories in our cricketing history", Modi tweeted.
India coach Ravi Shastri also paid tribute, tweeting a photo of Wadekar during his heyday as a cricketer.
"Sad moment for Indian cricket to lose one of its most successful captains. Shrewd to the core. Condolences to the entire family #TeamIndia #RIPAjitWadekar," Shastri tweeted.
In addition to his Test triumphs, Wadekar also served as India's first ODI captain and as manager of the team during Mohammad Azharuddin's tenure as captain in the 1990s.
The Board of Control for Cricket in India (BCCI) hailed his multifaceted career, which also included a stint as the chairman of selectors.
"With heavy heart, we bid adieu to Ajit Wadekar. The former India captain is no more. Cricketer, Coach, Manager and Chairman of Selectors - Mr Wadekar served Indian cricket in many different ways," the BCCI wrote on Twitter.