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A solution-processable organic–inorganic hybrid material composed of a polysiloxane urethane acrylate composite (PSUAC) was developed through a dual cross-linking mechanism and satisfies all the requirements for use as a gate dielectric for flexible organic thin-film transistors (OTFTs). PSUACs incorporate the urethane group for promoting adhesion to substrates and the acrylate group for enhancing the degree of cross-linking via a photo-curing reaction. Aluminium acetoacetate is introduced as a thermal curing agent that reacts with the silanols at the end of the PSUA resin, thus realizing a reliable dielectric that is barely affected by the slow polarization induced by moisture absorption. Thin films of the cross-linked PSUAC provided smooth surfaces with a root-mean-square roughness of <0.3 nm and which exhibited high breakdown voltages of >6.2 MV cm−1, while the capacitance was only slightly affected by …