Valverde's main goals for the 2016 season were the Ardennes classics, the Giro d'Italia and the Road Race at the Olympic Games in Rio. He started his season by taking the overall at the Vuelta a Andalucía in February. He out-powered the rest of the contenders, including Tejay van Garderen and Rafał Majka, on the climb up to the finish on the final stage. Valverde changed his initial plan of riding the Tour of Flanders and went to Tenerife to prepare for the Giro. He returned to competition by winning two stages and the overall at the Vuelta a Castilla y León which he chose to race instead of the Amstel Gold Race, a race still lacking from his palmáres. The following Wednesday he took his third consecutive La Flèche Wallonne victory and became the most prolific winner of the "smaller" Ardennes Classic with his fourth win. He showed his climbing prowess by controlling up until the last when he accelerated away from his rivals to take the victory. The Sunday following, he went out to repeat his Ardennes double from 2015 by securing another Liège–Bastogne–Liège win but he fell short and only managed to finish 16th.