Valverde, one of very few riders with major titles or podium finishes in both grand tours and one-day races, controlled the opposition in the mountains before securing the win in the 27.7-km time trial around Eibar on Saturday.
Overall, he beat fellow Spaniards Alberto Contador and Jon Izaguirre by 17 and 21 seconds respectively.
The 36-year-old will be the man to watch in the Ardennes classics that start next weekend with the Amstel Gold Race in the Netherlands.
Two races in Belgium then follow -- the Fleche Wallonne, which Valverde has won for the last three years, and Liege-Bastogne-Liege, which he has claimed on four occasions.
(Reporting by Julien Pretot; Editing by Ian Chadband)
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