The frictional properties of lithium compound grease (LCG) with different percentage compositions of few-layer graphene (FLG) were investigated, and the mechanisms of temperature and loading effects on LCG containing FLG are also considered. The concluding effect shows that 1 wt% FLG is more appropriate for friction and wear modifiers for lithium compound grease at elevated temperatures and less suitable at ordinary temperatures. Thickener chemisorption film, FLG layering film, and tribo-reaction film consisting of FeO(OH), Fe 2O 3, Fe 3O 4, Li 2O, and other oxides assist in the establishment of a lubricating boundary film on the friction interfaces lubricated with LCG containing FLG. The poor fluidity of lithium compound grease at low temperatures leads to poor dispersion of FLG, decreasing friction reduction capability. Under elevated temperature and low load condition, adding 1wt% FLG to LCG can only improve its wear-resistant property, the abrasion volume of steel plate reduced by 24.49%. Under elevated temperature and high load condition, adding 1wt% FLG to LCG can only enhance its anti-friction characteristics.. Conversely, FLG is unsuitable as an anti-friction and wear-resistant additive for LCG at low-temperature conditions.