Thermal spray coatings are used extensively for the protection and life extension of engineering components exposed to harsh wear and/or corrosion during service in aerospace, energy, and heavy machinery sectors. Cermet coatings applied via high-velocity thermal spray are used in aggressive wear situations almost always coupled with corrosive environments. In several instances (e.g., landing gear), coatings are considered as part of the structure requiring system-level considerations. Despite their widespread use, the technology has lacked generalized scientific principles for robust coating design, manufacturing, and performance analysis. Advances in process and in situ diagnostics have provided significant insights into the process-structure-property-performance correlations providing a framework-enhanced design. In this overview, critical aspects of materials, process, parametrics, and performance are discussed through exemplary studies on relevant compositions. The underlying connective theme is understanding and controlling residual stresses generation, which not only addresses process dynamics but also provides linkage for process-property relationship for both the system (e.g., fatigue) and the surface (wear and corrosion). The anisotropic microstructure also invokes the need for damage-tolerant material design to meet future goals.