Abstract: Ni2P supported catalysts exhibit high catalytic activities in hydrogenation reaction, of which the particle sizes of Ni2P active phases are the key influential factor. This research focus on the effect of chelators on the size of Ni2P particles over wrinkle silica nanoparticles (WSNs) by introducing chelating agents EDTA and NTA during impregnation process. The characterization results show that chelators modified catalysts possess smaller size of Ni2P particles than the unmodified Ni2P catalysts. Among all the synthesized catalysts, the EDTA modified Ni2PE(1.5)/WSNs catalyst possesses smallest average particle size of Ni2P, only 2.6 nm. Moreover, the Ni2P catalysts with the assistance of EDTA exhibits better catalytic activity than that of NTA under high reaction temperature, which can be ascribed to the strong bonding between EDTA and Ni. And the EDTA modified Ni2PE(1.5)/WSNs catalyst shows highest hydrogenation ability, almost reaching 100% decalin selectivity.