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Polymer dielectrics have been widely used in electrical and electronic systems for capacitive energy storage and electrical insulation. However, emerging applications such as electric vehicles and hybrid electric aircraft demand improved polymer dielectrics for operation not only under high electric fields and high temperatures, but also extreme conditions, for example, low pressures at high altitudes, with largely increased likelihood of electrical partial discharges. To meet these stringent requirements of grand electrifications for payload efficiency, polymers with enhanced discharge resistance are highly desired. Here, we present a surface-engineering approach for Kapton® coated with self-assembled two-dimensional montmorillonite nanosheets. By suppressing the magnitude of the high-field partial discharges, this nanocoating endows polymers with improved discharge resistance, with satisfactory discharge endurance life of 200 hours at a high electric field of 46 kV mm −1 while maintaining the surface morphology of the polymer. Moreover, the MMT nanocoating can also improve the thermal stability of Kapton®, with significantly suppressed temperature coefficients for both the dielectric constant and dielectric loss over a wide temperature range from 25 to 205 °C. This work provides a practical method of surface nanocoating to explore high-discharge-resistant polymers for harsh condition electrification.