"Villarreal and Valencia have reached an agreement under which Carlos Marchena will form part of the squad for the next three seasons," Villarreal said on their website.
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The Sevilla-born 31-year-old, who can play as a centre-back or defensive midfielder, played for Valencia for nine seasons, winning two league titles and one King's Cup.
He has made 62 appearances for Spain, scoring two goals, and was part of coach Vicente del Bosque's victorious squad at the 2010 World Cup in South Africa.
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