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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. 

Abstract Hydrogels and polydimethylsiloxane (PDMS) are complementary to each other, since the hydrophobic PDMS provides a more stable and rigid substrate, while the water‐rich hydrogel possesses remarkable hydrophilicity, biocompatibility, and similarity to biological tissues. Herein a transparent and stretchable covalently bonded PDMS‐hydrogel bilayer (PHB) structure is prepared via in situ free radical copolymerization of acrylamide and allylamine‐exfoliated‐ZrP (AA‐e‐ZrP) on a functionalized PDMS surface. The AA‐e‐ZrP serves as cross‐linking nano‐patches in the polymer gel network. The covalently bonded structure is constructed through the addition reaction of vinyl groups of PDMS surface and monomers, obtaining a strong interfacial adhesion between the PDMS and the hydrogel. A mechanical‐responsive wrinkle surface, which exhibs transparency change mechanochromism, is created via introducing a cross‐linked polyvinyl alcohol film atop the PHB structure. A finite element model is implemented to simulate the wrinkle formation process. The implication of the present finding for the interfacial design of the PHB and PDMS‐hydrogel‐PVA trilayer (PHPT) structures is discussed.