Due to its excellent specific strength, corrosion resistance, and biocompatibility, titanium alloy is often used as a biological implant material. In order to address the issues of low hardness and poor wear resistance of the Ti-25Nb-3Zr-2Sn-3Mo titanium alloy, a TiN/Sn coating with good biocompatibility was deposited on its surface using a new composite modification technology of surface mechanical strengthening + surface mechanical coating. By taking advantage of the wear resistance of TiN and the adhesiveness of Sn, a composite coating with corrosion-wear resistance was formed to improve its corrosion-wear resistance. Using TiN/Sn powders of different ratios (10% Sn, 20% Sn, 30% Sn, and 40% Sn) as media, the alloy was subjected to a combined strengthening treatment of surface mechanical attrition and solid-phase coating under a nitrogen atmosphere. The microstructure and mechanical properties of the composite-strengthened layer were tested by means of XRD, SEM-EDS, a nanoindentation tester, a white-light interferometer, and a reciprocating wear tester. Moreover, the corrosion-wear properties of the samples under different loads and electrochemical conditions were analyzed. The results show that the surface composite-strengthened layer of the alloy consisted of a TiN/Sn coating + a mechanical deformed layer. With an increase in the Sn content, the thickness of the TiN/Sn coating continuously increased, while the thickness of the mechanical deformed layer continuously decreased. The composite-strengthened layer had good comprehensive mechanical properties. In the SBF solution, the corrosion-wear resistance of the composite-strengthened samples improved; the degree of wear first decreased and then increased with the increase in the Sn content, and it reached the optimal value when the Sn content was 30%. Compared with the raw sample, the corrosion of the coating sample increased, but the wear significantly decreased. The corrosion-wear synergy factor κ value first increased and then decreased with the increase in the Sn content, reaching a maximum value at the 20% Sn content. This is the result of the combined effect of the corrosion resistance and wear resistance of the coating.