Deshmukh had turned critical and died of multiple organ failure at 2 pm. His family members, including his three sons, were by his side at his end time.
He was earlier undergoing treatment at Breach Candy hospital in Mumbai for about a week and had to be shifted to super-speciality Global hospitals on August 6 due to deterioration in his condition.
A team doctors, including noted liver transplant surgeon Dr Mohamed Rela, had put in their best efforts to save him. Deshmukh was on life-support systems.
Efforts to save him suffered a major setback after a brain-dead man whose liver and kidney were to be harvested and transplanted in Deshmukh, died hours before the operation yesterday night.
Congress president Smt. Sonia Gandhi referred Deshmukh’s passing away as a great loss to the party.
President Pranab Mukherjee and Prime Minister Manmohan Singh have also expressed grief; the national flag will fly at half-mast.
Maharashtra Chief Minister Prithiviraj Chavan said that he is shocked at the demise of Deshmukh and termed him as one of the tallest leaders from Maharashtra.
Deshmukh will be remembered as a grass root leader who was banked upon by his party as a master political strategist.
Deshmukh, who previously held the posts of Minister of Rural Development and Minister of Panchayati Raj and Minister of Heavy Industries and Public Enterprises. He was the chief minister of Maharashtra twice, from 1999 to 2003 and from 2004 to 2008.
On July 19, Deshmukh was in New Delhi for the presidential election.
Both houses of Parliament were adjourned as soon as the news of the Congress leader's demise came in.
Vilasrao will be cremated at his native Babhalgaon village in Latur district tomorrow, family sources said.
The mortal remains of the departed leader will be brought to Latur tomorrow and kept at his house in Babhalgaon from 9 am to 3 pm for people to pay their last respects, his brother Dilip Deshmukh, said.
The funeral procession will start at 3 pm and last rites would be performed at 4 pm, he said.