Wear resistance and optical properties are the key point for the application of titanium alloys as structural materials in the aerospace field. To enhance the wear resistance and optical properties of titanium alloys, a black plasma electrolytic oxidation (PEO) coating incorporating MoSi 2 nanoparticles was fabricated on the TC4 alloy via the PEO process, with the MoSi 2 nanoparticles being in situ doped into the coating. The doping of MoSi 2 nano-particles can effectively reduce the pore size of the PEO layer. The nPEO coating exhibited lower surface roughness than that of the PEO layer. The surface hardness of the nPEO coating increased to 42.5 HRC, significantly enhancing the wear resistance of the PEO layer (40.7 HRC). Furthermore, the PEO coatings exhibited better optical property compared to TC alloy, and the incorporation of MoSi 2 particles further improved the performance in most wavelength ranges. The infrared emissivity of the nPEO coating was 0.87, a dramatic increase from the 0.38 value of the TC4 alloy. This coating strategy effectively enhances the wear resistance and optical performance of TC4 alloy, which is critical for the surface design of titanium alloys used in aerospace applications.