Graded metal-to-ceramic coatings as thermal barrier coating (TBC) have been studied to improve the surface properties of the coating on high-temperature components. The atmospheric and low pressure plasma spray experiments are carried out with partially stabilized zirconia (YSZ and MSZ) and MCrAlY for mixing of functionally gradient materials. Especially, three-layer and five-layer graded TBCs are designed and produced to match gradually the material properties of a substrate and a top coating for reducing thermal stresses. A fully-saturated fractional factorial test is employed to determine optimum process conditions related to the thermal plasma generation, powder feeding, and substrate handling. Microstructural analysis using optical microscope and SEM, compositional analysis by XRD, bond strength test and thermal shock tests are carried out for material evaluation of fabricated TBCs. According to the results of material evaluation, the spray process is optimized for improving coating quality, and the proper raw materials are selected as a result of microstructural analysis. Especially, it is found that the durability and strain tolerance to thermal shock are remarkably increased by the gradation of TBCs and the improvement of graded TBC results from the fracture mechanism related to the vertical crack.