The ex-Army officer, Henry Worsley, 55, was 30 miles short of his goal of becoming the first person to cross the continent unaided.
His wife Joanna said In a statement, she felt “heartbroken sadness.” Worsley died of “complete organ failure”, she added.
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The ReMark Group, which was supporting Mr Worsley’s effort, said in a statement: “When Henry was picked up by Antarctic Logistics and Expeditions (ALE), he was suffering from exhaustion and dehydration.
“He was flown to a hospital in Punta Arenas [in Chile] where he was found to have bacterial peritonitis.
“This resulted in Henry undergoing surgery but in spite of all the efforts of ALE and medical staff, he succumbed.”
Peritonitis is inflammation of the peritoneum, the thin layer of tissue that lines the inside of the abdomen. According to the NHS, most cases come from injury or infection in another part of the body.
The plan was to cross the continent “unassisted and unsupported” – with no supply drops or help from dogs or any other source.
He had passed his target of raising £100, 000 for the Endeavour Fund, which helps injured and sick servicemen and women.
In a statement, the fund said it was “devastated” by news of Worsley’s death.
Worsley began the 1, 100-mile (1, 770km) coast-to-coast trek in November, pulling a sledge containing his food, tent and equipment. Before he left London, he told the BBC he expected to lose 12.7kg during the challenge.
He said his journey should take 75 days and he would take enough food for 80 days, adding: “I could make it last a bit longer.”
Asked if he was “mad” to take on the challenge, he said: “There is no black art to sliding one ski in front of the other.
“What will drive me on is raising money for these wounded soldiers.”