Beschreibung:
<jats:title>Abstract</jats:title><jats:p>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 <jats:italic>d</jats:italic><jats:sub>33</jats:sub> of 39 pC N<jats:sup>−1</jats:sup>, 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<jats:sup>−1</jats:sup>, ultra‐fast recovery time of 0.2 ms and stable operation capability when coupled with metal electrodes, confirming their applicability for reliable pressure sensor.</jats:p>