Lasma-sprayed thermal barrier coatings (TBCs) are gaining wide popularity and becoming more attractive for many industrial applications due to their high strength, thermal barrier/fatigue characteristics at elevated temperatures, resistance to chemical degradation, wear resistance, and environmental corrosion protection provided when coated on the surface of engineering components. To characterize the tribological properties of TBCs, a better understanding of their failure mechanisms and a thorough investigation of their performance are required. In this research, we used Taguchi-based grey relational analysis (GRA) to optimize the process parameters of various tribological characteristics of ceramic coatings applied via an atmospheric plasma spray process. Using Taguchi L16 factorial mixed-level experimental design, we also evaluated tribological characteristics such as wear loss and the coefficient of friction. Using GRA, we successfully performed a multiple output optimization and ranking of the control factors. Based on ANOVA results, we evaluated the significance of each process parameter and validated our findings in tests using the obtained optimum set of process parameters. Our study results will help to minimize wear loss and the coefficient of friction and to maximize TBC life.