Lignin is an abundant source of aromatics and depolymerization of lignin offers significant potential for the production of high quality chemicals. The selective hydrogenolysis of the C − O ether bond in lignin is an important strategy for the production of fuels and chemical raw materials. In our study, the catalytic hydrogenolysis of lignin model compounds (β-O-4, α-O-4 and 4-O-5 model compounds) over Ni3rdS.2-CS catalysts was investigated. Hence an array of 2D carbon nanostructures is Ni3rdS.2-CSs-XY derived catalysts were produced with different compositions at different temperatures (X = 0 mg, 0.2 mg, 0.4 mg, 0.6 mg and 0.8 mg; Y = 600 ° C, 700 ° C, 800 ° C and 900 ° C) were prepared and used for the hydrogenolysis of lignin model compounds and the depolymerization of alkaline lignin. The highest conversion of lignin model compounds (β-O-4 model compound) was up to 100%, and the yield of the corresponding ethylbenzene and phenol obtained could be 92% and, respectively3rdS.2-CSs-0.4-700 catalyst in iPrOH at 260 ° C without external H2. The 2D carbon nanostructure catalysts dispersed well on the surface of the carbon nanosheets, which facilitated the cleavage of the lignin ether bonds. The physico-chemical characterization studies were carried out using XRD, SEM, TEM, H2-TPR, NH3rd-TPD, Raman and XPS analyzes. Based on the optimal reaction conditions (260 ° C, 4 h, 2.0 MPa N2), various model compounds (β-O-4, α-O-4, and 4-O-5 model compounds) could also be effectively treated with hydrogen to produce the corresponding aromatic products. In addition, the optimal is Ni3rdS.2-CSs-0.4-700 catalyst could be performed for the next five consecutive cycling experiments with a slight decrease in the conversion of lignin model compounds.