He was 77 and is survived by his wife Rekha, two sons and a daughter. Wadekar was brought to a hospital in South Mumbai today where he was declared dead on arrival.
His last rites will be performed on Friday, a member of the Wadekar family, who did not wish to be named, told PTI.
"He had been critically unwell for some time and was seeking treatment for the same," read the statement from the Jaslok Hospital.
The aggressive batsman was a trailblazer in Indian cricket despite a mere 37 Test appearances, leading India to triumphs in England and the West Indies in 1971.
Wadekar scored 2,113 runs in his Test career, including one hundred, and was also the country's first ODI captain. He appeared in just two matches, though.
India lost both those ODIs against England, which prompted Wadekar to retire from international cricket in 1974.
The Mumbaikar went on to serve as India's manager in the '90s during Mohammed Azharuddin's captaincy. In his tenure as manager, India had finished semifinalists at the 1996 World Cup.
V sad news-Ajit Wadekar passing away-only Indn Capt to win 3 series in a row-2 away 1 at home-ALW was good contemporary-we had differences o opinion but always respected glory o Crkt-fine batsman & great close in catch-served Indn Crkt w/aplomb as player/Selectr/Coach-RIP Jeetu!— Bishan Bedi (@BishanBedi) August 15, 2018
#AjitWadekar sir .. such an iconic person..deeply saddened by his demise!! Sir was a father figure for me.. May his soul rest in peace! My Heartfelt Condolences to the family..@BCCI pic.twitter.com/xLMb2i82B2— Mohammed Azharuddin (@azharflicks) August 15, 2018
With a 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. pic.twitter.com/6zdFtleXB9— BCCI (@BCCI) August 15, 2018
Deeply saddened by the passing away of #AjitWadekar He was more than a coach to the entire team - a father figure and a shrewd tactician. My heartfelt condolences to his family and loved ones. He will be missed. Thank you Sir for the confidence shown in my ability! 🙏— Anil Kumble (@anilkumble1074) August 16, 2018
Ajit Wadekar’s impact on Indian cricket is immense. His contemporaries worshipped him, such was his aura. Found him to be a tough character as coach. Exceptional Indian cricketer... RIP Sir.🙏— Sanjay Manjrekar (@sanjaymanjrekar) August 15, 2018
Recorded this on my iPhone last Dec from Point in a friendly fixture. So glad I did. pic.twitter.com/XbdFGn4Izp
So many memories of Ajit Wadekar. None more powerful than leading India to series wins in 1971 in England and the West Indies. Much admired, much loved. Page in Indian cricket and in our memories.— Harsha Bhogle (@bhogleharsha) August 15, 2018
Deeply saddened to hear about the demise of Ajit Wadekar Sir. He was someone who was instrumental in bringing out the best in us during the 90s. We’ll always be grateful for his advice and guidance. Praying for strength for his family during this difficult time. 🙏 RIP pic.twitter.com/coSyac73ot— Sachin Tendulkar (@sachin_rt) August 16, 2018
Ajit Wadekar will be remembered for his rich contribution to Indian cricket. A great batsman & wonderful captain, he led our team to some of the most memorable victories in our cricketing history. He was also respected as an effective cricket administrator. Pained by his demise.— Narendra Modi (@narendramodi) August 15, 2018
Sad at the passing of Ajit Wadekar, one of Indian cricket’s finest left-handed batsman and captain during the iconic overseas test victories in 1971 in the Caribbean and England. Condolences to his family and to the cricket fraternity #PresidentKovind— President of India (@rashtrapatibhvn) August 15, 2018
He later went on to become the chairman of selectors as well. Wadekar is the only cricketer apart from Lala Amarnath and Chandu Borde to have served as captain, manager, and selector in Indian cricket.
But the feat that made him an icon was the Test wins in the West Indies and England.
In a side that included the likes of Sunil Gavaskar, G Viswanath, and Bishan Singh Bedi, Wadekar took over the captaincy from M A K Pataudi in 1971.
And he immediately etched his name in history books with India's Test triumphs in England and the West Indies.
Wadekar's first-class debut was in 1958 but he could make it to the Indian team only in 1966 and went on to earn the reputation of being an aggressive number three batsman.
However, he had just one Test hundred in his record -- a 143-run effort in Wellington -- which came in the 1968 tour of New Zealand.
The left-hander ended his Test career with 14 half centuries, four of those being 90-plus scores.
He was bestowed the Arjuna Award in 1967 and India's fourth highest civilian honour, the Padmashri, in 1972.