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Pentacene-based organic thin-film transistors with solution-process hafnium oxide (HfOx) as gate insulating layer have been demonstrated. The solution-process HfOx could not only exhibit a high-permittivity (kappa = 11) dielectric constant but also has good dielectric strength. Moreover, the root-mean-square surface roughness and surface energy (gammas) on the surface of the HfOx layer were 1.304 nm and 34.24 mJ/cm2, respectively. The smooth, as well as hydrophobic, surface of HfOx could facilitate the direct deposition of the pentacene film without an additional polymer treatment layer, leading to a high field-effect mobility of 3.8 cm2/(V middots) .