In our research described here gold-phase molybdenum disulfide (1T-MoS2)/graphite-phase carbon nitride (g-C3N4) composites were prepared by a simple solvent-thermal method to investigate their synergistic lubrication in poly-α-olefin lithium grease by the four-sphere mode. The growth of 1T-MoS2 on g-C3N4 nanosheets was demonstrated by scanning electron microscopy (SEM), X-ray diffractometry (XRD) and Fourier transform infrared spectroscopy (FTIR). Tribological tests showed that the best tribological performance of the poly-α-olefin grease was achieved when the concentration of 1T-MoS2/g-C3N4 was 3 wt%; the coefficient of friction and the diameter of the abrasion marks were reduced by 37.7% and 51.2%, respectively, compared with the pure grease. Investigating the wear marks by field emission scanning electron microscopy (FE-SEM) and elemental mapping analysis, it was found that the coupling between the liquid lubrication film and the solid friction film and the synergistic effect between 1T-MoS2 and g-C3N4 were important factors to improve the tribological performance of the poly-α-olefin grease. We, therefore, note this study is expected to promote the development of new, high-performance greases.