In this paper, MSH-C and MSH-GO composites were prepared by doping MSH with micron-sized few-layer graphene oxide (∼10 um) and nanoscale graphite (∼300 nm), respectively, during the hydrothermal synthesis process. Octadecyltrimethoxysilane (ODTMS) was used as a surfactant to disperse these two types of additives into the fully formulated oil. Tribological tests demonstrated that MSH-C exhibits much more superior tribological properties when compared to MSH-GO. The findings reveal that the oil sample containing 0.5 wt% MSH-C can effectively reduce wear volume (by approximately 26.4%) as compared to fully formulated oil and that the friction coefficient is decreased to ∼0.02. SEM, Raman, FIB-TEM, and TOF-SIMS characterizations and molecular dynamics simulation were used to investigate the tribological mechanism. A tribo-film composed of two layers of different compositions was formed on the worn surface of MSH-C, indicating the synergistic effect of MSH and graphite.