The CoCrFeNiTi_(1-x) Mo_x high-entropy-alloy coating was prepared using a powder presetting method. The work investigated the influences of Ti and Mo addition on the microstructure and properties of CoCrFeNi high-entropy alloys. The first-principles calculation showed that CoCrFeNiTi_(1-x) Mo_x was mainly composed of the FCC phase, BCC phase, and IMCs. The coating exhibited high hardness, and the mechanical stability of the high-entropy alloys of FCC and BCC phases was maintained when x = 0.5. The coating primarily consisted of FCC, BCC, σand CoTi2 phases when x ≤ 0.75. The coating primarily consisted of FCC, BCC, σand Co2Mo3 phases when x = 1. It exhibited high microhardness, elastic modulus, elastic stiffness, and wear resistance when x = 0.5. Its average microhardness, local elastic modulus, and elastic stiffness were 873.28 HV0.5, 265.5606 GPa, and 102.8008 GPa, respectively. Besides, COF and the wear mass loss were 0.7026 mm3 and 0.0410 mm3, respectively. The coating exhibited exceptional corrosion resistance with a self-corrosion voltage of −0.700 V and a self-corrosion current of 5.387e-007 A when x = 1. The results offer practical guidance for preparing high-entropy-alloy coatings with various advantages as well as a theoretical foundation for preparing such alloys by laser cladding.