This work proposes a modified activated carbon support, with defects and heteroatoms (N,P-ACs) by nitrogen and phosphorus doping to load non-noble nickel to catalyze aromatic compound hydrogenation. The Ni/N,P-ACs-900 (prepared at 900 °C) showed promising catalytic activity in liquid-phase 1,5-dinitronaphthalene hydrogenation with a 1,5-diaminonaphthalene yield of 95.8% under the mild condition of 100 °C, which is comparable to the commercial Pd/C catalyst. The nitrogen species were burned off at 900 °C, causing more defects for nickel metal loading, facilitating the interaction between the supports and the nickel metal, and resulting in highly dispersed metal particles. The computational study of the nickel binding energy has been conducted using density functional theory. It exhibits that the defects formed by heteroatom doping are beneficial to nickel anchoring and deposition to form highly uniform nickel particles. The phosphorus species in combination with the defects are suitable for H adsorption and dissociation. These results reveal that the heteroatomic doping on the active carbon shows significant effects in the hydrogenation of the liquid-phase aromatic compounds. These findings could provide a promising route for the rational design of aromatic compound hydrogenation catalysts to significantly decrease the cost by instead using noble metal catalysts in the industry.