In this paper, a series of the environmental-friendly aqueous PAI-MoS2-graphite bonded solid-lubricating coatings (BSLCs) are prepared depending on the design concept of the recombination of two-component lubricant and aqueous resin, and the mechanical strength and wear resistance of the coatings are deeply optimized by virtue of the synergy of the components of coatings. The experimental results demonstrate that the successful preparation of aqueous BSLCs greatly reduces the utilization of toxic organic solvents and is conducive to environmental protection and resource conservation. Doping an appropriate amount of graphite into the aqueous BSLCs is beneficial to maximize the promotion of the mechanical and tribological properties of the coating, and when the mass ratio of graphite to MoS2 (MRGM) is 0.3, the mechanical strength, friction reduction and wear resistance of the coatings display the comparable level as that of the organic-solvent based BSLCs. Based on the analysis of the variations of the morphology, structure and chemical composition of the wear scars, the corresponding active mechanisms on the mechanical and tribological properties of the coating are investigated in depth.