Organic–inorganic polyvinylpyrrolidone–silicon dioxide–3-(trimethoxysilyl) propyl methacrylate (PVP–SiO2–TMSPM) hybrid solutions have been synthesized using the sol–gel process with different amounts of TMSPM as coupling agent and equivalent amounts of PVP and SiO2. Hybrid solutions were deposited on p-type Si(111) substrates using the spin coating technique, as a gate dielectric material for use in thin-film transistors. The structural properties of the samples were investigated using Fourier-transform infrared spectroscopy and x-ray diffraction analysis. Atomic force microscopy and scanning electron microscopy techniques were applied to study the topography and morphology of the hybrid thin-film samples. Current–voltage (I–V) curves, capacitance–voltage (C–V) measurements, and the electrical properties of the organic hybrid thin-film gate dielectrics were also studied in a metal–insulator/polymer–semiconductor structure. According to the results, the JGS curves in terms of VGS showed gate leakage current densities small enough for use as gate dielectric material at interface layers. At VDS = 30 V, in the saturation region, IDS curves in terms of VGS presented higher charge carrier mobility (lFET,S = 0.0584 cm2 s1 V1) due to lower dielectric constant (k = 11.43) in the sample with 0.05 weight ratio of TMSPM compared with other samples with different weight ratios of TMSPM.