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Abstract: A research on the design, synthesis, and characterization of novel cross-linked polymer organic–inorganic hybrid materials as gate insulators for organic thin-film transistors (OTFTs) with vanadyl-phthalocyanine as the organic semiconductor is presented. The hybrid films (0.5–1.2μm thick) can be easily prepared by sol–gel technology and fabricated by spin-coating a mixture of zirconium n-butoxide sol with a side-chain triethoxysilane-capped polyurethane solution in ambient conditions, followed by curing at low temperatures (∼120°C) and cross-linking under UV light. OTFTs with this film as gate insulator were achieved with good processability, high charge-carrier mobility of 0.56cm2/Vs, surface roughness of around 0.49–0.59nm, ultralow threshold of −6V, and ultralow leakage of 0.24mA. Hybrid films with various compositions were investigated, and the results showed that the field-effect mobility of the OTFTs was dominated by the high dielectric constant component ZrO2. The result indicated that these hybrid materials are promising candidates for the exploration of devices using OTFTs. [Copyright &y& Elsevier]