Nowadays, the advent of pressure sensors for intelligence terminal devices and skin‐inspired electronics has trigged rapid development of flexible, sensitive, and transparent sensing materials. Piezo‐active poly(vinylidene fluoride) (PVDF) is emerging as a promising candidate for sensing components due to the flexible and transparent features. However, the inherent weak piezo‐activity and consequently low sensitivity of PVDF remains a challenge for its sensing applications. Herein, ionic liquids ([EMIM]Cl) additive combined with a composition‐gradient multilayered architecture design are employed to hardness the piezo‐response of PVDF. The resultant composites present ultra‐high piezoelectric coefficient d33 of 39 pC N−1, which is 2.78 times that of PVDF. Meanwhile, the transparent ILs dopant enables the composites with superior transparency (87%). With notable advantages of high transparency and piezoelectricity, the ILs/PVDF composites exhibit high sensitivity of 0.0423 V N−1, ultra‐fast recovery time of 0.2 ms and stable operation capability when coupled with metal electrodes, confirming their applicability for reliable pressure sensor.
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