The current discussion of the application of dark-field X-ray microscopy (DFXM) to thin-film neuromorphic systems begins with VO2operando switching devices. The goal of this section is to lay out the applicability of DFXM to thin film systems while simultaneously providing information on the structural properties of the voltage switching in these devices based on VO2. A brief overview of the problems of conventional structural probes. The results of this study are then presented with a brief interpretation of the results as they apply to the further development of neuromorphic devices. Finally, future pathways as they apply to neuromorphic-device structure and DFXM on thin films are also briefly discussed.