NiCrAlY-PSZ graded materials with two different gradients were synthesized using the plasma spray technique. Their microstructure, thermal and frictional response were evaluated, and the response was compared to that of single layered composite materials. The hardness and frictional properties of PSZ could be successfully optimized by an addition of small amount of NiCrAlY. The results of testing revealed the potential of ceramic/metallic materials systems and can be used to further optimize the spraying process of composite/graded structures subjected to contact damage at high temperatures. The study also revealed new tribo-effects that can be encountered in potential applications of graded structures.