A series of core-shell structural hydrodenitrogenation (HDN) catalyst supports, using H-Beta zeolite nanoparticles as the core and tunable mesoporous materials SBA-16 thin film thickness as shell, were designed and controllably synthesized. The corresponding Ni2P catalyst were prepared, and their catalytic performances were tested for quinoline HDN. It was found that the high external surface area provided by the mesoporous shell layer of the core-shell catalyst favored the formation of Ni2P nanoparticles with more uniform particle size. The Py-IR result indicates that the SBA-16 shell thickness plays an important role in influencing the ratio of the amount of Bronsted and Lewis acid sites on the catalyst. The H2-TPR results indicates that the introduction of core-shell structure can adjust the metal-support interactions (MSI) of materials. The core-shell support with suitable shell thickness (70 nm) exhibits a wide pore structure, large surface area and sufficient amounts of Lewis and Bronsted acid sites. These properties contribute to the formation of tiny and size homogeneous (4.6 nm) Ni2P nanoparticles. Smaller Ni2P particles present more active sites, which increases catalytic activity. The Ni2P/H-Beta@SBA-16–2 catalyst with the most suitable shell thickness exhibited a higher reaction rate constant and TOF for HDN reaction of quinoline.