The nanocomposite gate insulating film of a pentacene-based thin film transistor was deposited by inkjet printing. In this study, utilizing the pearl miller to crumble the agglomerations and the dispersant to well stabilize the dispersion of nano-TiO2particles in the polymer matrix of the ink increases the dose concentration for pico-jetting, which could be as the gate dielectric film made by inkjet printing without the photography process. Finally, we realized top contact pentacene-TFTs and successfully accomplished the purpose of directly patternability and increase the performance of the device based on the nanocomposite by inkjet printing. These devices exhibited p-channel TFT characteristics with a high field-effect mobility (a saturation mobility of ̃0.58 cm2 V−1 s−1), a large current ratio (>103) and a low operation voltage (<6 V). Furthermore, we accorded the deposited mechanisms which caused the interface difference between of inkjet printing and spin coating. And we used XRD, SEM, Raman spectroscopy to help us analyze the transfer characteristics of pentacene films and the performance of OTFTs.