A novel antiwear filler Nano-MOS2 capped PBO fiber was synthesized via an economical one-pot hydrothermal method and further be used to reinforce the tribological behavior of TPI/PEEK matrix at high temperature. Experimental results revealed that the as-prepared PBO-MOS2 fiber had stronger interfacial adhesion with the blended matrix(30%TPI/PEEK), when compared to the untreated PBO fiber. Therefore, this enhancement could be beneficial to stress transfer from the matrix to fiber during friction process. In addition, further experiment indicated that the mechanical property, thermal stability and lubrication performance of the as-prepared composite also has been improved. Especially, the PBO-MOS2 reinforced TPI/PEEK composite showed excellent wear resistance and friction-reducing capacity at high temperature. The COF and wear rate reduced 22.9% and 61.1%, respectively, at 200 degrees C.