The operating conditions of functional materials usually involve varying stress fields resulting in either intentional or undesirable structural changes. Complex multiscale microstructures, including defects, domains and new phases in functional materials can be induced in situ by mechanical loading, providing fundamental insight into their deformation process. The resulting microstructure, if induced in a controllable fashion, can be used to tune the functional properties or to enhance their performance. In-situ nanomechanical testing conducted in (Scanning) Transmission Electron Microscopes (STEM/TEM) provides a PROGRESS REPORT 2critical tool for understanding the microstructural evolution in functional materials. In this report, select results from a variety of functional materials systems will be presented in the context of newly developed multi-modal experimental capabilities to demonstrate the impact of these techniques.