Spanish league leaders Real Madrid can increase their advantage at the top when they host Athletic Bilbao in a match postponed from the ninth round.
The result was harsh on Villarreal who were pressing for a winning goal when a bad defensive error gifted Barca their second goal of the game late on Saturday night.
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Marco Asensio, Nacho Fernández, Vinícius Júnior and Ferland Mendy all scored to give Madrid its fourth straight straight victory in all competitions.
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Barcelona remained in ninth place in the league and with their horizon of success narrowing to simply securing a top-four finish to ensure their spot in the Champions League.
Barcelona reserve-team coach Sergi Barjuan will temporarily lead the squad until they find a permanent replacement for Koeman.
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The 18-year-old Fati made his first start for Barcelona after a long injury layoff on Sunday, scoring a goal and earning his team a penalty as the Catalan club halted its losing streak by rallying to beat Valencia 3-1.
Luis Suarez and Thomas Lemar set up goals for each other as Atletico Madrid dealt Barcelona another harsh helping of life without Lionel Messi.
Wearing the No. 10 jersey that used to belong to Lionel Messi, Ansu Fati made a triumphant return from a long injury layoff on Sunday, scoring a goal in 3-0 win over Levante.
The draw on Saturday gave Madrid a three-point lead over Sevilla at the top of the table.
Victor Laguardia scored with a header off a corner four minutes into the match, giving Alavés its first points of the season
Barcelona was held to a 0-0 draw by Cádiz in the Spanish league on Thursday, extending its winless streak to three matches and adding pressure on coach Ronald Koeman.
It was Madrid's fourth straight league win, taking Carlo Ancelotti's team back to the top of the standings with 16 points from six matches, two points ahead of defending champion Atletico Madrid.
The Uruguayan scored two late goals to give Atlético Madrid a 2-1 win at Getafe in the Spanish league on Tuesday, ending the team's two-match winless streak.
The first of three consecutive matches in the Santiago Bernabeu sees Carlo Ancelotti's side look to build on their positive start to the season.
In desperate move to find goal, Koeman sent in defender Gerard Pique to play as a striker in the closing minutes as the match ended 1-1.
Vinicius Jr levelled for Madrid in the 86th minute with his shot also taking a big deflection to wrong-foot Valencia keeper Giorgi Mamardas.
Griezmann will get another chance to win back the hearts of Atlético’s faithful on Saturday against the unbeaten Athletic Bilbao.
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