Club officials did not give a reason for the coaching staff departing but said they hope to announce an interim or permanent coach “in the coming hours”.
The 50-year-old joined the club in 2013, helping win promotion to La Liga and leading Villarreal to three straight top-six finishes. They reached the Europa League semi-finals last season, losing to Liverpool, and finished fourth in the league, earning a place in the Champions League play-offs.
Villarreal play Monaco next Wednesday, with the return leg six days later – and start their league season at Granada on Saturday.
The news comes a day after the club also lost the striker Roberto Soldado for six months owing to a cruciate ligament tear. The 31-year-old’s injury means the summer signing Alexandre Pato is their only fit striker.
A club statement said: “Tests have confirmed Soldado suffered an anterior cruciate ligament tear and a torn external meniscus in his right knee. He will undergo surgery in the next few days.”
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