The 60-year-old departs with the Yellow Submarine sitting third in LaLiga with four games remaining, a position that guarantees a return to Europe's elite competition next term. His exit follows weeks of uncertainty over his future, with talks over a new deal failing to result in an agreement.
In a statement on Monday, Villarreal paid tribute to a coach who has overseen more matches than any other in the club's history. Marcelino will finish with 298 games in charge across his two spells, along with a record 145 victories.
"Villarreal CF and Marcelino García Toral will part ways at the end of the season," the club said. "He will end his second stage at the entity after achieving Champions League qualification for the second consecutive year - for the first time in the club's history.
"Thank you, from the bottom of our heart, Marce. Thank you for everything you have given to this club and to these fans."
Marcelino first managed Villarreal between 2013 and 2016, guiding them back to the top flight, before returning in 2023 and immediately restoring their competitiveness at the top end of LaLiga. Last season's fifth-place finish was followed by another strong domestic campaign, even as Villarreal struggled in Europe and exited the Champions League at the league phase.
His broader managerial CV includes a Copa del Rey triumph with Valencia in 2019 and a Spanish Super Cup win with Athletic Bilbao in 2021, while he has also previously coached Sevilla and Marseille. He has recently been linked with a possible move to the Premier League.
Villarreal are already preparing for life after Marcelino, with Rayo Vallecano manager Inigo Perez lined up as the leading candidate to take over, although final details of that appointment are yet to be resolved.
The club plan to honour Marcelino in their final LaLiga fixture against Atletico Madrid, which is also set to serve as a celebration of their Champions League qualification with supporters at Estadio de la Ceramica.
