We reported on organic thin-film transistors (OTFTs) with high dielectric constant polymer, poly(2,2,2-trifluoroethyl methacrylate) (PTFMA), as the gate dielectric. In top-contact OTFTs, the field-effect mobility was enhanced by applying a dielectric buffer layer poly(alpha-methylstyrene) to the bare PTFMA. After improving interfacial affinity within the active layer/dielectrics, deposited pentacene grain size and device performance were enhanced dramatically. The corresponding mobility, threshold voltage, and on/off current ratio were 0.70 cm(2) V(-1) s(-1), -10.5 V, and 5.4x10(5), respectively. The moderately improved interface also suppressed the hole-trapping effect, which led to less hysteresis and minimized threshold voltage shift.