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Ferroelectric organic field-effect transistor nonvolatile memories (Fe-OFET-NVMs) offer attractive features for future memory applications, such as flexible and wearable electronics. Polymer semiconductor-based top-gate Fe-OFET-NVMs possess natural advantages in the device structure and processing manufacturing, compared to small-molecule semiconductor-based bottom-gate Fe-OFET-NVMs. However, their performances, such as mobility and operating voltages, should be further improved to be comparable to those of the latter. In this Letter, we develop a route to achieve high-performance top-gate Fe-OFET-NVMs, by employing a polymer semiconductor channel and self-organized ferroelectric/dielectric gate insulators, which were processed by a solution spin-coating technique. The optimal Fe-OFET-NVM exhibits a high mobility of 1.96 cm2/V s on average, a reliable endurance over 400 cycles, a stable retention capability over 6 × 104 s, and a life more than one year. Furthermore, the operating voltage of the Fe-OFET-NVM is reduced to ±20 V by scaling down the thickness of the ferroelectric/dielectric gate insulator. The whole performances of our memories are comparable to or better than those of the previous Fe-OFET-NVMs. [ABSTRACT FROM AUTHOR]