"Scans this morning confirm fractured navicular. End of the Vuelta for me," Froome posted on his official Twitter account.
Froome's hopes of becoming just the third man to win the Tour and the Vuelta in the same year were realistically ended on Wednesday as he injured his foot whilst crashing on the daunting mountainous 138km ride through Andorra and fell over seven minutes behind general classification leader Fabio Aru.
The 30-year-old was hoping to emulate Frenchmen Jacques Anquetil (1963) and Bernard Hinault (1978) by completing the Tour-Vuelta double and was very much in contention before Wednesday's stage, dubbed as one the hardest in the Vuelta's 80-year history with four category one and a special category climb.
Froome got off to the worst possible start, though, as a crash early in the day left him needing crutches to walk at the end of the stage.
"Knocked sideways into a barrier and stone wall today. Further scans in the morning but start unlikely as I can't walk without crutches," he posted on Twitter on Wednesday.
Knocked sideways into a barrier & stone wall today. Further scans in the morning but start unlikely as I can't walk without crutches #LV2015— Chris Froome (@chrisfroome) September 2, 2015
"Really appreciate all the messages of support, I did my best to hang in there today as best I could with the hope of continuing."
Froome's withdrawal is the latest blow for the tour organisers in a race that has been mired by dangerous crashes and controversy.
The team time trial on the first stage didn't count towards the overall classification as it was deemed too dangerous.
Italian Vincenzo Nibali, one of just six men to have won all three Grand Tours, was then disqualified on the second stage for being towed by his Astana team car.
Belgian rider Kris Boeckmans remains in an induced coma after a serious crash on the eighth stage, which also forced general classification contenders Dan Martin and Tejay van Garderen to retire.
On the same day, stage three winner Peter Sagan was run over by an auxiliary motorcycle forcing him to withdraw and bringing a stinging response from his Tinkoff-Saxo team.
Tinkoff-Saxo were further incensed when another one of their riders, Sergio Paulinho, was also forced to retire after being hit by a TV motorcycle on Wednesday.
Oleg Tinkoff, the Russian entrepreneur who owns the team, has even threatened to withdraw from the race in protest at the safety provided to riders by the Amaury Sport Organisation (ASO) who run the event.
"I'm considering now to take the team off the #Vuelta2015 . Boycott #ASO for this. They pay us NO money for the race and even damage riders," he posted on Twitter.