Low-voltage and high-performance pentacene thin-film transistors with a hybrid gate dielectric consisting of ultrathin PVP (8 nm) and a high-kappa HfLaO (20 nm) have been demonstrated. The hybrid gate dielectric exploits the advantages of both dielectrics, i.e., a good interface between the organic dielectric and channel material as well as the insulating properties of the inorganic metal-oxide, resulting in very low leakage current, hysteresis-free behavior, superior drain-current drivability, and successful operation at -2 V. The superior device performance is attributed to good intermolecular ordering and the large grain size of the pentacene channel layer formed on the hybrid dielectric.