Organic field‐effect transistors (OFETs) with good flexibility and low operating voltage, are of great meaning for the low power stretchable and wearable electronic devices. The operating voltage and flexibility are easily affected by the dielectric layers in the OFETs. Bilayer dielectrics comprising both high‐ and low‐permittivity (k) insulating polymers, have been reported. The flexible bilayer dielectrics can combine the advantages of both insulating polymers, which are high charge carriers from low‐k polymers and low operating voltage from high‐k polymers. However, the effect of film thicknesses in the bilayer dielectrics on the OFET performance is seldom investigated. Here, bilayer dielectrics comprising high‐k polyvinyl alcohol (PVA) and low‐k polymethylmethacrylate (PMMA) were fabricated. And PVA/PMMA bilayers with three different PVA film thicknesses are carefully investigated. The 300 nm PVA/100 nm PMMA bilayer dielectric makes the pentacene OFETs show the highest hole mobility of 1.24 cm2V−1s−1 and the corresponding inverters give a high voltage gain of 40 and a noise margin of 2.3 V (77% of 1/2 VDD) at low operating voltage of 6 V. Both the pentacene transistors and the inverters still work properly under bending radium of 5.85 mm, proving the good prospects of the PVA/PMMA bilayer dielectric in practical applications.