Villarreal are reportedly hopeful of appointing former Manchester City boss Manuel Pellegrini as their new manager after being left stunned by Marcelino's exit on the eve of the new season.
The 50-year-old, who was overlooked for the Spain job recently despite being favourite, is said to have stepped down due to several disagreements with club officials.
Marcelino's departure comes just days before a crucial Champions League playoff first-leg tie against AS Monaco, with Eurosport reporting that the Yellow Submarine are now looking to bring Pellegrini on board.
Pellegrini previously managed Villarreal between 2004 and 2009, famously leading the club to the semi-final stage of Europe's showpiece competition, as well as a third-place finish in La Liga eight years ago.
Should the Chilean turn down the offer, it is claimed that Villarreal will instead turn to an interim coach until a permanent successor can be found.