This study reports the preparation and characterization of polyimide/Ta(2)O(5) nanocomposite films as insulators for organic thin-film transistors (OTFTs). The degree of imidization, thermal, electrical, and surface properties of the nanocomposite films were characterized as a function of Ta(2)O(5) precursor contents. The nanocomposite films, with controlled/comparable insulator electrical characteristics and surface properties, have been found to enhance dielectric constant compared to pristine polyimide films, which resulted in improved pentacene TFT performance by a factor of 2-3 with carrier mobility values as high as 0.38 cm(2)/Vs. (C) 2011 Elsevier B.V. All rights reserved.