A cardanol-based polymer, poly(2-hydroxy-3-cardanylpropyl methacrylate) (PHCPM), was utilized as the gate dielectric of an organic field-effect transistor (OFET). PHCPM has good surface properties, appropriate gate dielectric characteristics, and good compatibility with solution-processed semiconducting polymers. The electrical properties of an FET that was prepared with natural resource-based PHCPM as a gate dielectric layer and solution-processed poly[2,5-bis(3-dodecylthiophen-2-yl)thieno[3,2-b]thiophene] (PBTTT) as a semiconducting layer were investigated on flexible substrates. The flexible PBTTT-OFET device with the PCHPM gate dielectric exhibited high mobility and reliable performance, even in the bending state, without significant hysteresis.