Rapid chemical functionalization of additives and efficient determination of their optimum concentrations are important for designing high-performance lubricants, especially under multi-additive conditions. Herein, chemically functionalized graphene (FGR) and carbon nanotubes (FCNTs) were rapidly prepared by microwave-assisted ball milling and subsequently introduced into grease as additives. The tribological properties of the additives in grease at different concentrations and ratios were measured using a four-ball test. A reliable artificial neural network (ANN) model was established according to a few test results. Subsequently, the optimal concentration of multiple additives in the grease was predicted using a genetic algorithm and experimentally validated. The results indicated that the introduction of FGR (0.14 wt %) and FCNT (0.16 wt %) improved the antifriction and anti-wear performance of the base grease by 25.66 and 29.34%, respectively. The results of the ANN model analysis and friction interface characterization indicate that such performance is principally attributed to the synergistic lubrication of the FGR and FCNT.