This paper presents a compound laser surface modification strategy to enhance the tribological performance of biomedical titanium alloys involving femtosecond laser nitriding and femtosecond laser texturing. First, high-repetition-rate femtosecond pulses (MHz) were used to melt the surface under a nitrogen atmosphere, forming a wear-resistant TiN coating. Subsequently, the TiN layer was ablated in air with low-repetition-rate femtosecond pulses (kHz) to create squared textures. The effects of the combined nitriding and texturing treatment on bio-tribological performance was investigated. Results show that compared with the untreated samples, the single femtosecond laser nitriding process increased the surface hardness from 336 HV to 1455 HV and significantly enhanced the wear resistance of titanium, with the wear loss decreasing from 9.07 mg to 3.41 mg. However, the friction coefficient increased from 0.388 to 0.655, which was attributed to the increased hardness, roughness within the wear scars, and the formation of hard debris. After combined treatment, the friction coefficient decreased to 0.408 under the optimal texture density of 65%. The mechanisms for the improvement in friction behavior are the reduction in contact area and the trapping of hard debris.