Villarreal have appointed Marcelino as manager following the departure of Jose Rojo Martin just two months after taking charge, the Spanish club said late on Monday.
Rojo Martin, known as 'Pacheta', parted ways with Villarreal on Friday, with Director of Football Miguel Angel Tena leading the side in their 3-1 defeat at Atletico Madrid on Sunday.
Marcelino, who has signed a deal until 2026, also managed Villarreal from 2013 to 2016 and guided them to the Spanish top flight.
The 58-year-old helped Villarreal achieve three top-six finishes and a Europa League semifinal in his final season.
Marcelino last coached Ligue 1 side Olympique de Marseille.
Villarreal are 14th in LaLiga with 12 points from 13 matches. They next host 12-placed Osasuna on November 26.