The self-assembled hybrids were synthesized as a kind of filler with the function of reinforcing and lubricating, by which can improve its dispersion in the matrix, and enhance the interfacial adhesion with the matrix. However, the effect of the amount of grafting on the hybrid properties is still unclear. In this study, a series of antiwear hybrids with different grafting amount were synthesized and further be used to reinforce thermoplastic polyimide matrix. The method of comparative analysis had been applied to analyze the microstructural morphology, thermal property, mechanical property, and high temperature tribological behavior of these composites. The results indicated that with the increasing grafting amount of MoS₂ on the PBO fiber surface in a certain range, the integrated performance of the composite increases.