Metal-oxide charge trapping memory (CTM) integration into amorphous and organic flexible devices encounters challenges due to high-temperature treatment. Our approach enhances memory performance via room-temperature oxygen plasma treatment, subtly adjusting surface band alignment without changing the original material structure and surface roughness. Infiltration of oxygen plasma induces band alignment bending, creating a barrier for charge trapping. The device with oxygen plasma treatment exhibits an impressive 19.06 V memory window and a charge trapping density of 3.58 × 1013/cm2. In comparison, the memory window of untreated device only has 5.56 V, demonstrating that oxygen plasma treatment significantly improves memory characteristics. The charge retention rate exhibits outstanding stability, potentially reaching 94% after a decade. It should be noted that careful control during plasma treatment is crucial to maintaining optimal memory effects. This facile, efficient technique, applicable to various oxide layers, offers a way for future advancements in metal-oxide CTM technology.