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.