Villarreal have set their sights on Real Madrid goalkeeper Diego Lopez and Deportivo La Coruna midfielder Aldo Duscher, according to reports in Spain.
Depor full-back Joan Capdevila is to join Villarreal in the summer, while Roberto Ayala will also move to El Madrigal from Valencia.
Villarreal are now looking to strengthen their squad in other areas, and have targeted Lopez as their ideal choice in goal.
Lopez is back-up for Iker Casillas at Real but remains highly rated and has been linked with several clubs over the past 12 months.
Argentine Duscher was tipped to leave Depor in the January transfer window but decided to wait until the end of the season when he will be out of contract.
Villarreal president Fernando Roig explained: "We need to reinforce every position for the team to return to Europe."