Villarreal has fired coach Luis Garcia Plaza after it won only one of its nine matches under his command.
The team is second-to-last in the Spanish league standings, five points from safety.
Villarreal lost at Valencia 3-0 in its last league game, a result that extended the team’s winless streak to eight matches in all competitions.
It will host Espanyol in the league on Sunday.
The club did not immediately appoint a replacement for Plaza, who arrived in December after Javi Calleja was fired.
The team’s only win under Plaza was against Spartak Moscow in the group stage of the Europa League, in his first game in charge. The team drew four straight matches after that, including against Real Madrid at home in the league, then lost three of its next four in all competitions.
Villarreal is the first team to have changed coaches twice this season.