This study presented the desirability function based on Taguchi designed experiments to solve multiple responses statistical optimal problems for the tungsten carbide/cobalt (WC-Co) coatings of high-velocity-oxygen-fuel (HVOF) processes. The eight control factors based on L18 arrays were conducted and the multi-responses of wear-resistant coatings such as hardness, deposited thickness and wear rate were evaluated simultaneously in the desirability-based experiments. Based on desirability analysis, the optimal settings have been identified, and the impacts of control factors are determined by analysis of variance on the multi-responses. Further, a confirmation run was conducted to validate the tests. Experimental results have shown that the hardness increased by 16.61% and the deposited thickness improved by 10.50%, while the wear rate decreased by 34.03%. It was clear that confirmation tests are greatly improved by way of the desirability-based multi-responses on HVOF WC-Co experiments, and these findings achieved the desired values on wear-resistant coatings. The proposed procedure was applied at HVOF sprayed WC-Co experiments, and the implementation results demonstrated its feasibility and effectiveness to maximize hardness, make a target of deposited thickness value and minimize wear rate by a HVOF.