Atletico Madrid had earlier turned up the heat on champions Barcelona when they fought back to secure a 2-1 win at home to Athletic Bilbao.
Atletico’s battling victory put them level at the top on 35 points with Barca, who surrendered a 2-0 advantage and were held 2-2 at home by Deportivo La Coruna on Saturday, their second consecutive draw after last weekend’s 1-1 stalemate at Valencia.
Barca are ahead on goal difference, while Real are five points adrift in third after Roberto Soldado scored against his former club to give Villarreal, who are a point off fourth spot with 27, the spoils at the Madrigal.
Real fielded their famous attacking trident of Cristiano Ronaldo, Gareth Bale and Karim Benzema but could not make a host of chances count and the defeat heaps more pressure on under-fire coach Rafa Benitez.
At Villarreal, midfielder Jonathan Dos Santos had already hit a post before Soldado, a graduate of Real’s youth academy, struck to put the home side ahead in the eighth minute.
Real laid siege to the Villarreal goal in the second half but despite a string of efforts they only managed one on target and slipped to a third league defeat of the season.
They were a shadow of the side that demolished Malmo 8-0 in the Champions League on Tuesday, with Ronaldo and Benzema particularly wayward.
“We were not switched on at the start,” Real centre back Pepe told Spanish television.
“We are still in the fight but it’s true that we have to start games differently and better,” added the Portugal international.
Former England defender Gary Neville is still without a win in two games since taking over as Valencia coach after his new club had a man sent off and needed an Eibar own goal to rescue a 1-1 draw at the modest Basque side.
Valencia, Eibar and Bilbao each have 21 points in eighth, ninth and 10th respectively.
