Villarreal and coach Jose Rojo Martin have parted ways two months after he took the job, the Spanish club said on Friday.
Martin, known as 'Pacheta,' joined Villarreal in September after the departure of Quique Setien.
Villarreal have had a disappointing start to the season with three wins in 12 matches and sit 13th in the standings on 12 points.
Pacheta only led the team in eight La Liga matches, three Europa League games and one Copa del Rey clash.
His final game in charge was a dramatic 2-1 victory over Israeli side Maccabi Haifa in the Europa League on Thursday, secured by two late goals.
Miguel Angel Tena, director of football, will lead the team when they travel to Atletico Madrid on Sunday.