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Here, we copolymerize a monomer containing naphthyl group with 2-hydroxyethyl methacrylate (HEMA) and glycidyl methacrylate (GlyMA) in various molar ratio to obtain copolymers as functional gate dielectric layers of thin-film transistors (TFTs). Using naphthyl-containing molecule to have similar chemical structure with pentance to adjust the grain size of semiconductor. The results indicated that the semiconductor grains size decreased as molar percentage of naphthyl-containing compound in the polymer structure increased, which could also affect the charge carrier mobility of the pentacene thin-film transistors (TFTs). Therefore, this can be a promising manner to fabricate pentacene TFTs with a high charge carrier mobility by using functionalized dielectric layers to obtain uniform grain size of the pentacene semiconductor. Image 1 • Novel polymer insulating materials containing naphthyl group were designed for OTFTs. • The effect of the content of naphthyl group in the polymers on the mobility was studied. • The larger and more uniformed gain size of pentacene was achieved on the designed polymer surface. • A strategy for the design of polymer as gate dielectric was proposed to improve the mobility of OTFTs. [ABSTRACT FROM AUTHOR]