Villarreal missed their chance to stay in touch with Real Madrid at the top of the Primera Liga when they went down 2-0 at Valladolid on Sunday.
The defeat kept Manuel Pellegrini's side level with Barcelona on 28 points in third spot in the table and four adrift of leaders Real, who won 3-1 at home to Racing Santander on Saturday.
Villarreal went into the game after winning three of their last four games but never looked comfortable against a determined Valladolid side who put them under real pressure in midfield and hit them hard on the break.
The home side went in front in the 18th minute when unmarked striker Joseba Llorente powered a header past Villarreal keeper Sebastian Viera after he met a fine cross from winger Sisi.
Former Villarreal striker Victor made it 2-0 early in the second half when he poked home from close range after a slick passing move involving Llorente and winger Jonathan Sesma.
Atletico Madrid moved up to fourth spot, just a point behind Barca and Villarreal, after goals from Diego Forlan and Raul Garcia earned them a 2-0 win away to struggling Real Betis.
Forlan put Atletico ahead 11 minutes before the break when he controlled a clever lofted pass from strike partner Sergio Aguero with his chest and shot low past keeper Ricardo.
Betis pushed hard in the second half and were denied an equaliser only after a great double save from Atletico keeper Leo Franco who blocked fierce shots from Leandro Somoza and Rafael Sobis.
Garcia made sure of the win when he drilled home left-footed from the edge of the area after his first shot had rebounded off a defender.
Defeat for Betis meant they remain second from bottom, two points behind Deportivo Coruna who lost 2-1 at home to Osasuna.
Ronald Koeman's Valencia, who exited the Champions League this week, continued their poor run of form when they slumped to a 3-0 at home to Athletic Bilbao that kept them in sixth spot in the table on 24 points.
A superb curling free kick from midfielder Fran Yeste and a second-half double from Fernando Llorente earned the Basque side their first win at the Mestalla in 20 years and prompted angry scenes from the home crowd.
Michael Laudrup's Getafe notched their fourth win in five games after a double from striker Braulio earned them a 2-1 comeback victory over bottom club Levante which lifted them up to 10th place.