Thermal spraying is a directed melt spray deposition process, in which inorganic particles in the diameter range of 1-100 microns are heated, melted (in some cases partially), propelled and impacted onto a prepared substrate. A rapid sequence of events occurs including: melting, impact (in some cases shock), spreading and rapid solidification, all of which take place in microsecond timescales, enabling materials synthesis from extreme conditions. The sprayed coating is resultant from successive assemblage of such microscale impacted droplets (splats) producing mesoscale thick films or coatings. The coatings thus produced are anisotropic, layered structures with multiple length scales of material character and interfacial defects, with concomitant implications on properties. The layered assembly also imparts gradients in residual stresses within the thickness of the coating. These effects are in large part deemed “unintentional” and incorporated in many applications with limited manipulation.