Abstract: A novel and highly active nitrogen-doped porous carbon-supported nickel catalyst Ni@N-PC was successfully developed by a thermolysis of nickel-based zeolitic imidazolate frameworks growing on both sides of graphitic carbon nitride and used for catalyzing hydroconversion of isopropanol soluble portion from ultrasonic extraction of high-temperature coal tar (ISP_HTCT). The active nickel nanoparticles were mainly encapsulated on the top of carbon nanotubes and partially dispersed on the surface of carbon nanosheets. Naphthalen-1-ol was used as a model compound to investigate the catalytic hydroconversion activity under different reaction conditions and reveal the mechanism for catalytic hydroconversion. The ISP_HTCT and catalytic hydroconversion products of ISP_HTCT (ISP_CHCP) were analyzed with gas chromatograph/mass spectrometer. The results show that 70% of naphthalen-1-ol was converted at 160 °C and completely converted at 200 °C for 120 min, and the ISP_HTCT was greatly upgraded. A total of 180 organic compounds including 33 nitrogen-containing organic compounds, 11 sulfur-containing organic compounds and 39 oxygenates were identified in ISP_HTCT, while no obvious nitrogen-containing organic compounds, sulfur-containing organic compounds and oxygenates were detected in ISP_CHCP, indicating the excellent performance of Ni@N-PC for heteroatom removal. All the alkenes, cyclenes and alkynes were saturated and the majority of arenes were converted to cyclanes by catalytic hydroconversion over Ni@N-PC, which exhibited high catalytic hydrogenation activity.