• A direct SAM treatment on the polar polymer gate dielectric without any preprocess is introduced. • A hysteresis-free OFET with a high mobility of 1.51 cm 2 V −1 s −1 was achieved. • An ultra-flexible OFET was fabricated and presented a stable electrical performance under deformations. Surface treatment for the polymer gate dielectric plays a significant role in achieving the high-performance flexible field-effect transistors. In this work, the direct SAM treatment on the polar polymer gate dielectric is introduced and the effects on the electrical performance of OFETs are investigated. After an appropriate SAM treatment for the polar polymer dielectric, the mobility can be improved and the hysteresis and interfacial trap states are decreased obviously. Moreover, the SAM treated polymer dielectric is used to achieve the ultra-flexible OFET successfully, with a stable electrical performance under various deformations. These results demonstrate that the direct SAM treatment on polar polymer dielectric is a promising strategy for the high-performance flexible organic transistors, presenting the huge potential for the next-generation flexible electronics.