We demonstrate that the endurance and compatibility of organic ferroelectric films can be impressively enhanced by a strategy of inhibiting charge injection and high-energy ions diffusion through inserting a large-band-gap ${\mathrm{Al}}_2{\mathrm{O}}_3$ interfacial layer between the organic ferroelectric films and electrodes. The $\mathrm{Pt}/{\mathrm{Al}}_2{\mathrm{O}}_3/\mathrm{P}\left(\mathrm{VDF}\text{−}\mathrm{TrFE}\right)/{\mathrm{Al}}_2{\mathrm{O}}_3/\mathrm{Al}$ capacitor exhibited remarkable fatigue-recovery characteristics with a durability of up to ${10}^{11}$ cycles, which is attributed to the sandwiched ${\mathrm{Al}}_2{\mathrm{O}}_3$ layer, suppressing the charges injection and slowing down the dehydrofluorination process within the P(VDF-TrFE) films. Additionally, the ${\mathrm{Al}}_2{\mathrm{O}}_3$ layer effectively impedes the damage of ion diffusion during the following film deposition, improving the compatibility of P(VDF-TrFE) films with other metal electrodes and semiconductor materials. A ZnO-based memory transistor modulated by ${\mathrm{Al}}_2{\mathrm{O}}_3/\mathrm{P}\left(\mathrm{VDF}\text{−}\mathrm{TrFE}\right)/{\mathrm{Al}}_2{\mathrm{O}}_3$ back gate was successfully fabricated which shows a robust on/off ratio of ∼100 over ${10}^{11}$ cycles.

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• Electric polarization
• Ferroelectricity
• Organic semiconductors
• Polymers