The preparation of a low shearing shell on the surface of carbon spheres (CS) is an attractive strategy to improve the lubrication properties of CS. In this study, core–shell structural C@Ag particles were prepared using CS as the hard core and Ag nanoparticles as the soft shell. Then, the additives were mixed with Polyalphaolefin 20 to prepare the C@Ag core–shell-enhanced lithium complex grease (C@Ag-LCG). The physicochemical properties, corrosion resistance, and tribological behaviors of LCGs were investigated. C@Ag-LCG exhibited the best high-temperature resistance and colloidal stability compared with the CS-enhanced lithium complex grease (LCG) and pure LCG. The dropping point and oil separation rate of 0.05 wt% C@Ag-LCG were 255 °C and 2.36 %, respectively. The tribological behavior of greases was tested using a four-ball friction tester, and the main damage mechanism was abrasive wear. The C@Ag additive reduced the average friction coefficient and wear spot diameter by 27.17 % and 26.12 %, respectively. The improved properties were attributed to the synergistic lubrication of hard CS core and soft Ag shell with the rolling, filling, and self-repairing effects, C@Ag deposit films and the self-lubricating oil film, as well as the thickener film and the tribochemical film at the frictional interfaces.