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Abstract To satisfy continual demands for higher performance dielectrics in multi‐layer ceramic capacitors and related microelectronic devices, novel characterization methods are necessary for mapping materials properties down to the nanoscale, where enabling materials developments are increasingly relevant. Accordingly, an atomic force microscopy‐based approach is implemented for characterizing insulator performance based on the mapping of discharging dynamics. Following surface charging by biasing a conducting tip contacting a dielectric surface, consecutive non‐contact Kelvin force surface potential mapping (KPFM) reveals charge dissipation via exponential decay. In barium titanate (BTO) thin films engineered with distinct microstructures but identical thicknesses, discharging rates vary by up to a factor of 2, with smaller grain size correlating to longer dissipation times, providing insight into optimal microstructures for improved capacitor performance. High‐resolution potential mapping as a function of time thereby provides a route for directly investigating charge injection and discharging mechanisms in dielectrics, which are increasingly engineered down to the nanoscale and have global implications given the trillions of such devices manufactured each year. 

Abstract The organic insulator–metal interface is the most important junction in flexible electronics. The strong band offset of organic insulators over the Fermi level of electrodes should theoretically impart a sufficient impediment for charge injection known as the Schottky barrier. However, defect formation through Anderson localization due to topological disorder in polymers leads to reduced barriers and hence cumbersome devices. A facile nanocoating comprising hundreds of highly oriented organic/inorganic alternating nanolayers is self‐coassembled on the surface of polymer films to revive the Schottky barrier. Carrier injection over the enhanced barrier is further shunted by anisotropic 2D conduction. This new interface engineering strategy allows a significant elevation of the operating field for organic insulators by 45% and a 7× improvement in discharge efficiency for Kapton at 150 °C. This superior 2D nanocoating thus provides a defect‐tolerant approach for effective reviving of the Schottky barrier, one century after its discovery, broadly applicable for flexible electronics.