Pentacene thin-film transistors (TFTs) with a high dielectric constant gate insulator, titanium silicon oxide (TiSiO2), were fabricated on flexible polyethylene naphthalate films coated with indium tin oxide layers. In order to define the device characteristics, the thickness dependence of the gate dielectric properties was studied. The pentacene TFT with a 132-nm-thick TiSiO2 film showed high performance with a threshold voltage of −0.88V, an inverse subthreshold slope of 317mV/decade. From the current-voltage characteristics, the field-effect mobility was obtained, resulting in an impressive mobility of 0.67cm2∕Vs at an operating voltage as low as −5V.