Froome had been hoping to become the third man to win the Tour de France and Vuelta a Espana in the same year but he crashed early on stage 11.
It was won by Spain's Mikel Landa from the Astana Pro Team. Italian team-mate Fabio Aru took the overall classification lead.
"It was a real demonstration of strength and I'm really happy to be in the leader's jersey," said Aru.
"There's still 10 stages to go and so we'll take things day by day but we'll try to defend it."
Dutchman Tom Dumoulin had been in the red jersey at the start of the day but he finished almost three minutes back at the end of a punishing mountain stage.
Spaniard Landa had surged clear of a splintered field around nine kilometres from the steep finish into Cortals d'Encamp, while team-mate Aru came second and Froome's Team Sky team-mate Ian Boswell third.
Froome limped home almost nine minutes behind the stage winner and afterwards team-mate Geraint Thomas said that the Tour de France winner had injured a foot, knee and shoulder.
Team Sky later tweeted that the team leader had gone to hospital for an X-ray on his foot after struggling to put weight on it.
The 30-year-old had started the day in eighth place, one minute, 18 seconds off the lead, he is now seven minutes 30 seconds behind the leader with his victory hopes in tatters.
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