Ethylenediamine (en) and diethylenetriamine (DETA) intercalated zinc sulfides (ZnS) ZnS(en) 0.5 and ZnS(DETA) 0.5 were prepared by solvothermal method. An SRV-V high frequency reciprocating tribometer was used to investigate the tribological properties of ZnS(en) 0.5 and ZnS(DETA) 0.5 as lithium-based grease additives. The morphologies and elemental distributions of the worn surfaces were characterized by means of scanning electron microscopy (SEM), three-dimensional (3D) optical profiler and X-ray energy dispersion spectroscopy (EDS). The results from tribological experiments illustrate that ZnS(en) 0.5 and ZnS(DETA) 0.5 could effectively improve the load-carrying capacity and anti-wear and friction reduction properties of the lithium grease. The larger interlayer spacing was helpful to enhance the anti-wear property. The anti-wear performance of the grease containing ZnS(DETA) 0.5 was obviously better than that of ZnS(en) 0.5 .