Substitute Enes Unal scored twice in the final nine minutes as Villarreal dealt a major blow to Atletico Madrid's title hopes with a 2-1 win.
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Villarreal have suspended defender Ruben Semedo without pay after he was arrested and charged with attempted murder and robbery.
Semedo faces charges of attempted murder, kidnap, robbery and unlawful possession of a firearm.
A spokeswoman for Spain's Guardia Civil told ESPN FC that the arrest had been made after an official complaint by the alleged victim of an incident.
Cristiano Ronaldo scored two penalties as Real Madrid eased some of the pressure on coach Zinedine Zidane with a 4-1 victory over Valencia.
Cedric Bakambu is poised to join Chinese Super League club Beijing Guoan after a deal was struck to rescind his contract at Villarreal.
Villarreal piled the pressure on under-fire Real Madrid coach Zinedine Zidane as they snatched a 1-0 win over the struggling La Liga champions.
Villarreal have agreed a deal to sign Colombian striker Roger Martinez from Chinese Super League club Jiangsu Suning.
Barcelona seized on the second-half dismissal of Dani Raba to beat Villarreal 2-0 and restore their five-point lead at the top of La Liga on Sunday.
Atletico Madrid are still undefeated and in fourth after notching their fifth draw, a disappointing 1-1 result at home versus Villarreal.
Atletico Madrid could only manage a 1-1 draw at third-division club Elche as Spain's leading clubs struggled in the Copa del Rey on Wednesday.
Villarreal have promoted Javi Calleja as their new head coach following the sacking of Fran Escriba on Monday.
Xabi Prieto was on the scoresheet in his 500th appearance for Real Sociedad as the Basque side saw off Villarreal 3-0 to make it two wins from two.
A late penalty from captain Jose Morales gave Levante a 1-0 win over Villarreal in their La Liga return at Ciutat de Valencia.
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