Two sets of plasma spray processing conditions were utilized in the investigation of graded layers, consisting of NiCrAlY and PSZ. Following the optimization of the plasma spray parameters and particle characteristics, the deposition efficiencies (DEs) of various powder species was examined. Selection of the best suited powders for coating production were selected based on the DE results. The base DEs were corrected by conducting the analyses using pre-deposited substrates as targets. Individual mixed coating layers were prepared and their compositions confirmed by image analysis. The effects of standoff distance and substrate temperature were also seen to have an effect on the DE and thus the coating formation. It is suggested that two-feeder, single injector plasma processing may not be the optimal method for the formation of FGMs.