The Yellow Submarine beat Almeria 1-0 thanks to a goal from Jonathan Pereira, which meant they moved just behind Elche into second.
Villarreal cannot now be caught as they get ready for a second spell in La Liga after their memorable 12 year stint which ended last season.
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The reputation of the Premier League means it is the most popular and one of the most watched leagues in the world.
Five English clubs will compete in the last sixteen of the Champions League for the first time ever as Liverpool, Manchester United, Manchester City, Chelsea and Tottenham face some difficult away matches.