Over the last decade there has been an explosion in terms of available tools for sensing the particle spray stream in thermal spray processes. This has led to considerable enhancement in our understanding of process reproducibility and reliability. Despite these advances, the linkage to coating properties has continued to be an enigma. This is partially due to the complex nature of the build-up process and the associated issues with measuring properties of these complex coatings. In this paper, we identify critical issues in processing-structure-property relations particularly with respect to the linkage to particle properties. Our goal is to demonstrate an integrated strategy, one that combines particle state sensing, with process mapping and extracting coating properties in situ through the development of robust and advanced curvature-based techniques. These techniques allow estimation of coating modulus, residual stress and, non-linear response of thermal sprayed ceramic coatings all within minutes of the deposition process. Finally, the integrated strategy examines the role of process maps for control of the spray stream as well as tailoring properties of thermal spray coatings. Examples of such studies for yttria-stabilized zirconia thermal barrier coatings are discussed.