An investigation into the dependency of the formation of functionally graded materials (FGMs) on process variables was carried out. The initial stage of the investigation involved a complete analysis of the plasma spray parameters used in the fabrication of an FGM constructed of NiCrAlY and partially stabilized zirconia (PSZ). In flight particle temperature, velocity and trajectory data were gathered for individual powders, as well as mixtures of the particle species, over a range of spray parameters. This data was combined with material specific properties such as flowability, apparent density, particle morphology and size distribution. The end result of the studies allowed for size matching of the particle species so as to ensure both species were molten at the nominal spray distance and possessed coincident impact velocities. Following the initial investigation, two spray conditions were selected for further analysis. Individual layers of specific powder mixture ratios were deposited as well as a complete FGM structure. The resulting structures were then compared based on their deposition efficiencies, porosity levels, compositional homogeneity and microstructures.