This study reports on the Grey relational system, with a statistical experiment to enhance the quality characteristics of yttria stabilized zirconia (ZrO2/8%Y2O3)coatings made by a plasma-sprayed process. The eight control factors were designed in an L18 factorial orthogonal array experiment, and the effects of the control parameters on the surface properties were critically evaluated in the experiments. The characteristic terms- surface roughness, porosity, hardness, and wear volume in the sprayed ZrO2/8%Y2O3 coatings through the optimization- were studied comparatively. A grey relational system, based on the Taguchi orthogonal experiment for optimizing multi-responses in the modified properties, was reported. In addition, the influence of control factors on the grey relational system for spraying processes was investigated by analysis of variance. In addition, a confirmation experiment was conducted. Experimental results have shown that the hardness increased by 31.19%, while the surface roughness decreased by 40.67%, the porosity was reduced by 53.53%, and the wear rate improved by 24.21%. It is clear that the quality characteristics for plasma sprayed coatings are greatly improved through grey relational analysis, and that these findings achieved the desired values in regard to the modified properties.