Calcium sulfonate complex greases (CSCG) have proven to be a sustainable alternative to lithium complex greases, which still require appropriate additives to deliver lubrication performance benefits under extreme working conditions such as heavy load, high speed, and high temperature. The anti-wear and friction reducing properties of CSCG enhanced by two-dimensional MoS 2 nanosheets (2D MoS 2) with a narrow lateral size and thickness distributions were evaluated by a four-ball tribometer. The results showed that the CSCG with 0.6 wt.% 2D MoS 2 performs best, with a 56.4% decrease in average friction coefficient (AFC), 16.5% reduction in wear scar diameter (WSD), 14.3% decrease in surface roughness, and a 59.4% reduction in average wear depth. Combining SEM-EDS images, Raman, and X-ray photoelectron spectra, it is illustrated that the physical transferred film and tribo-chemical film consisting of MoS 2, Fe 2O 3, FeSO 4, CaCO 3, CaO, and MoO 3 were generated on the worn surface, which improves the lubrication performance of CSCG considerably.