High-performance organic thin-film transistors (OTFTs) with a nanoparticle composite dielectric layer have been demonstrated. The dielectric layer consists of cross-linked poly-4-vinylphenol (PVP) and high-dielectric titanium dioxide (TiO 2) nanoparticles. Because of the nanosize of TiO 2, it disperses well in the organic solvent, which makes it possible to use solution-processable methods to prepare the dielectric layer. OTFTs with pentacene as the semiconducting layers have been demonstrated; it was found that the OTFTs with the nanocomposite dielectric layer have higher field-induced current than that of conventional devices because the dielectric constant of the gate insulator is increased. This finding opens an interesting direction for the preparation of high-performance OTFTs without complicated sputtering of high-k dielectric materials.