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For advanced electronic device applications including printable, flexible organic electronics and bioelectronics, it is crucial to develop novel dielectric materials with high dielectric strength and low-temperature processability compatible with plastic substrates for producing flexible and low-voltage organic thin-film transistors (OTFTs). Herein, we report the facile fabrication of rationally designed, high-capacitance hybrid gate dielectric films for low-voltage OTFTs on plastic substrates via a room-temperature solution process. To create room-temperature-processed gate dielectrics with high dielectric strength, we designed organic-inorganic hybrid gate dielectric films by including ZrOx networks as inorganic high-k oxide materials for obtaining large capacitance and 1,6-hexanediol diacrylate as a bifunctional UV cross-linking agent and a flexible organic component for increasing the density and flexibility of films and ensuring room-temperature processability. The UV cross-linked ZrOx-based hybrid composite films with a 15 nm thickness showed excellent dielectric properties with a leakage current density of ∼10−6 A/cm2 and a capacitance of 640 nF/cm2. The film surfaces were modified with hydrophobic self-assembled monolayers to match the surface energy of organic semiconductors for enhancing the OTFT performance. The utility of the hybrid dielectrics for flexible OTFTs was demonstrated by realizing pentacene TFTs on plastic substrates with a low operating voltage at –2.5 V, a high on/off current ratio of 105, a threshold voltage as low as –0.7 V, and a hole mobility up to 0.47 cm2 V−1 s−1, which are comparable to those performed on Si substrates. [ABSTRACT FROM AUTHOR]