A novel process for improving tar yield through catalytic depolymerization of a typical lignite was put forward. The catalytic depolymerization of the lignite over CoCl2 and ZnCl2 catalyst in different concentrations were investigated by a Gray-King apparatus. The optimal catalyst concentrations of CoCl2 and ZnCl2 catalyst that could obtain the highest tar yield was achieved, by which the tar yield increased about 20.3% and 6.6% compared with that of the raw coal, respectively. Different with the traditional catalytic pyrolysis process for which the tar yield decreased, more tar was produced by the catalytic depolymerization method. The GC × GC-MS analysis showed that the components of alkanes and two-ring aromatics in tar increased dramatically with the addition of the optimal CoCl2 and ZnCl2 catalyst. The Raman measurement revealed that more large aromatic ring systems ( > 6 rings) were formed in the char from depolymerization with catalyst and the elemental analysis showed that the hydrogen content decreased slightly. The gas products analysis reflected the contents of methane showed an obvious decrease. All of this reflects that more fragments and small free radicals cracked were enhanced by catalysis in the catalytic depolymerization process, thereby leading to an enhancement of the tar formation possibilities.