Al-TUD-1 (AT) material was successfully prepared via sol-gel method and modified by phosphoric acid. A series characterization of NiMoP/AT catalysts results indicated that after the addition of phosphoric acid, the NiMoP/ AT-x series catalysts still retained the large specific surface area and pore structure, which accommodated the active metals for better dispersion. Phosphoric acid could effectively ameliorate the acidity of catalyst and modulate metal-support-interaction (MSI), then the molybdenum species were sulfided to transform into octahedral MoS2 active species with higher degree of sulfurization and dispersion degree. Catalytic performances of different catalysts were estimated using Dibenzothiophene (DBT) and Fluid Catalytic Cracking (FCC) diesel as feedstock, The NiMoP/AT-2 exhibited the maximal DBT hydrodesulfurization (HDS) efficiency of 98.6 % and the highest values of HDS (99.1 %) and hydrodenitrogenation (HDN) (98.5 %) efficiencies for FCC diesel.