On 19 April 2012, after helping Olympiacos renew its league supremacy, Valverde announced his decision to leave due to family reasons. On 3 December he returned to Spanish football by being appointed at Valencia until the end of the campaign, replacing the fired Mauricio Pellegrino; his first game occurred five days later, a 1–0 win at Osasuna, and the second match, against the same opponent for the Spanish cup, brought another triumph at the Reyno de Navarra (2–0).