The 28-year-old was found with his brother Andre, 25, after their vehicle came off the road in the western city of Zamora, the Spanish Civil Guard said.
The incident in which Diogo Jota and Andre Silva died was possibly caused by a tyre blowing out while the car was overtaking.
Paying tribute to the forward Liverpool manager Arne Slot said "the sense of shock is absolute", adding "Diogo was not just our player. He was a loved one to all of us."
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