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Scarcity of the antisolvent polymer dielectrics and their poor stability have significantly prevented solution-processed ultraflexible organic transistors from low-temperature, large-scale production for applications in low-cost skin-inspired electronics. Here, we present a novel low-temperature solution-processed PEI-EP polymer dielectric with dramatically enhanced thermal stability, humidity stability, and frequency stability compared with the conventional PVA/c-PVA and c-PVP dielectrics, by incorporating polyethyleneimine PEI as crosslinking sites in nonhydroxyl epoxy EP. The PEI-EP dielectric requires a very low process temperature as low as 70°C and simultaneously possesses the high initial decomposition temperature (340°C) and glass transition temperature (230°C), humidity-resistant dielectric properties, and frequency-independent capacitance. Integrated into the solution-processed C8-BTBT thin-film transistors, the PEI-EP dielectric enables the device stable operation in air within 2 months and in high-humidity environment from 20 to 100% without significant performance degradation. The PEI-EP dielectric transistor array also presents weak hysteresis transfer characteristics, excellent electrical performance with 100% operation rate, high mobility up to 7.98 cm 2  V -1  s -1  (1 Hz) and average mobility as high as 5.3 cm 2  V -1  s -1  (1 Hz), excellent flexibility with the normal operation at the bending radius down to 0.003 mm, and foldable and crumpling-resistant capability. These results reveal the great potential of PEI-EP polymer as dielectric of low-temperature solution-processed ultraflexible organic transistors and open a new strategy for the development and applications of next-generation low-cost skin electronics.

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Highly Stable Nonhydroxyl Antisolvent Polymer Dielectric: A New Strategy towards High-Performance Low-Temperature Solution-Processed Ultraflexible Organic Transistors for Skin-Inspired Electronics