We report on the fabrication of pentacene-based thin-film transistors (TFTs) with a 230nm-thick double polymer dielectric composed of 30nm-thin low-k poly-4-vinyphenol (PVP) and 200nm-thick high-k poly(vinylidene fluoride/trifluoroethylene) [P(VDF–TrFE)] dielectric on polyethersulfone (PES) films. Our 230nm-thick double (high-k/low-k) polymer showed a good dielectric strength of ∼2MV/cm, a high capacitance of 26nF/cm 2 with k=∼7. Based on this double polymer dielectric, our flexible pentacene TFT displayed a high saturation mobility of 1.22cm 2 /Vs, a threshold voltage of −2.5V, and on/off ratio of 10 3 , stably operating under −5V.