Aseries of CoMo/ZrO2-Al2O3 catalysts with different contents of ZrO2 were prepared and characterized through XRD, XPS, NH3-TPD, H2-TPR, HR-TEM, and N2 adsorption–desorption technologies. The performance of the catalysts for low-temperature coal tar (LTCT) hydrocracking reaction was investigated. The interaction between active metals and Al2O3 was weakened with the introduction of ZrO2, which increased the MoS2 content and the stack layer number of MoS2 slabs to further promote the catalytic performance. At the same time, the amount of acid sites increased with an increasing ZrO2 content. When the ZrO2 content reached 32％, the pore volume of the catalyst decreased signiifcantly. This phenomenon reduced the content of MoS2 and the stack layer number of MoS2 slabs, which were not conducive to improving the catalytic performance. The catalyst containing 24％of ZrO2 exhibited the best catalytic performance for hydrocracking reaction, with the residue conversion and the total yield of gasoline and diesel fractions reaching 60.64％and 66.54％, respectively, which could fulifll the requirements for hydrocracking LTCT.