We numerically find values of four process input parameters, namely, the argon flow rate, the hydrogen flow rate, the powder feed rate, and the current, that yield the desired mean particles’ temperature and the mean particle velocity (collectively called mean particles’ characteristics, or MPCs) in an atmospheric plasma spray process just before the particles arrive at the substrate to be coated. Previous studies have shown that the coating quality depends upon the MPCs. The process is simulated by using the software, LAVA-P-3D, that provides MPCs close to their experimental values. Thus, numerical rather than physical experiments are conducted. We first use the design of experiments to characterize the sensitivity of the MPCs to process parameters. We then identify relationships between the significant input parameters and the MPCs by using two methods, namely, the least squares regression and the response surface methodology (RSM). Finally, we employ an optimization algorithm in conjunction with the weighted sum method to find optimum values of the process input variables to achieve desired values of the MPCs. The effects of weights assigned to the objective functions for the temperature and the velocity, and the difference in using the regression and the RSM model have been studied. It is found that these values of the process parameters provide MPCs within 5% of their desired values. This methodology is applicable to other coating processes and fabrication technologies such as hot forging, machining and casting.