A highly efficient bimetallic nanoparticles (BMNPs) catalyst was reported, Pd1Ni4/AC, consisting of Pd1Ni4 BMNPs supported on active carbon, shown excellent catalytic performance and stablity in hydrodeoxygenation (HDO) of vanillin. HDO of vanillin and various aldehydes with high efficiency and selectivity could be achieved at low H-2 pressure (2 bar) under mild conditions in the presence of the BMNPs catalyst, no obvious decrease on catalytic performance was observed after eight cycles. The superior catalytic performance of the Pd1Ni4/AC catalyst was mainly attributable to the synergetic electronic effect between Pd and Ni, which showcased the great potential of BMNPs in the catalysis field.