Novel polyurethane containing terphenyl groups were designed and synthesized as gate insulators to induce the crystallization of p-sexiphenyl(p-6P) for organic thin-film transistors (OTFTs). Different sizes and shapes of p-6P grains were measured by atomic force microscopy (AFM), and results showed that the large size of p-6P grain can improve the performance of OTFTs. About 900nm thick films can be easily fabricated by spin-coating under ambient conditions, followed by curing at UV irradiation for 10min. OTFTs with this film as gate insulator were found to have good processability, a high charge-carrier mobility of 1.1cm 2 /Vs, a threshold voltage of −25V, and an on/off current ratio>10 5 . The result indicated that this material is a promising candidate for the exploration of devices using OTFTs.