Villarreal have announced Marcelino will leave his role as head coach at the end of the season.
The 60-year-old's second spell at the club will come to an end when they host Atletico Madrid on the final day of the campaign, on May 24.
Marcelino was appointed head coach for a second time at Villarreal in November 2023, following an initial spell between January 2013 and August 2016.
By the time he leaves, Marcelino will have managed a club-high 298 games across all competitions, while his 145 wins are also the most of any Villarreal coach.
The Yellow Submarine defeated Levante 5-1 last time out, securing back-to-back seasons in the Champions League for the first time in their history.
"Villarreal CF and Marcelino Garcia Toral will part ways at the end of the current campaign," a club statement read.
𝐎𝐅𝐅𝐈𝐂𝐈𝐀𝐋 𝐒𝐓𝐀𝐓𝐄𝐌𝐄𝐍𝐓: @Marcelino
— Villarreal CF English (@VillarrealCFen) May 4, 2026
Villarreal CF and Marcelino García Toral will part ways at the end of the current campaign
Thank you from the bottom of our hearts, Marce. Thank you for everything you have given to this club and its supporters. We wish you all… pic.twitter.com/suRr0Xrslt
"Thank you from the bottom of our hearts, Marce. Thank you for everything you have given to this club and its supporters. We wish you all the best in your future sporting projects."
During this current spell with Villarreal, Marcelino has won 58 of his 117 matches at the helm, with 52 of those victories coming in 97 LaLiga games.
His side struggled in the Champions League this term, finishing 35th in the league phase after picking up just one point from eight games.
Villarreal have secured their spot in the top four in LaLiga, however, and they still have a slim chance of finishing second above Real Madrid.