In this study, a high-K material, aluminum oxide (AlOx), as the dielectric of organic field-effect transistors (OFETs) was used to reduce the threshold and operating voltages, while focusing on achieving high-electrical-stability OFETs and retention in OFET-based memory devices. To achieve this, we modified the gate dielectric of OFETs using polyimide (PI) with different solid contents to tune the properties and reduce the trap state density of the gate dielectric, leading to controllable stability in the N, N’-ditridecylperylene-3,4,9,10-tetracarboxylic diimide (PTCDI-C13)-based OFETs. Thus, gate field-induced stress can be compensated for by the carriers accumulated due to the dipole field created by electric dipoles within the PI layer, thereby improving the OFET’s performance and stability. Moreover, if the OFET is modified by PI with different solid contents, it can operate more stably under fixed gate bias stress over time than the device with AlOxas the dielectric layer only can. Furthermore, the OFET-based memory devices with PI film showed good memory retention and durability. In summary, we successfully fabricated a low-voltage operating and stable OFET and an organic memory device in which the memory window has potential for industrial production.