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As the core component of wearable electronic devices, flexible energy storage materials play an irreplaceable role. At present, it is still a challenge to prepare flexible electrode materials with high energy density. In this paper, a polyaniline‐based composite flexible conductive hydrogel (PPG‐P) with a two‐level conductive network is successfully prepared by a secondary induced assembly in situ polymerization method. The special conductive structure greatly promotes the efficiency of charge transfer and the utilization of electroactive substances, so that PPG‐P exhibits excellent electrochemical performance. In a three‐electrode system, PPG‐P has a mass‐specific capacitance as high as 989 F g−1 (0.5 A g−1). After 1000 charge and discharge cycles, the capacitance retention is 87%. Symmetrical flexible supercapacitors based on PPG‐P have high specific capacitance (176 F g−1/0.5 A g−1) and high energy density (15.6 Wh kg−1). After 1000 cycles of constant current charge and discharge, the capacitance maintains 78.1%. The preparation of PPG‐P with a hierarchical structure demonstrates the possibility of achieving high energy density in flexible electrode materials, which has great application potential in the development of energy storage elements in wearable devices. [ABSTRACT FROM AUTHOR]

With the development of alternatives to traditional fossil energy and the rise of wearable technology, flexible energy storage devices have attracted great attention. In this paper, a polyaniline/poly(acrylamide‐sodium acrylate copolymer) hydrogel (PASH) with high flexibility and excellent electrochemical properties for flexible electrodes is fabricated by freeze‐thaw‐shrink treatment of a highly water‐absorptive hydrogel, together with in‐situ polymerization of aniline at a low aniline concentration (0.1 mol L−1). The PASH exhibits a conductivity of 4.05 S m−1 and an elongation at break of 1245%. The freeze‐thaw‐shrink treatment greatly improves the electrochemical performance and stability of the conductive PASH. The area specific capacitance of PASH reaches 849 mF cm−2 and the capacitance maintains 89% after 1000 galvanostatic charge–discharge cycles. All the raw materials are conventional industrialized materials and no additional templating agent is needed during the entire synthesis process. This study provides a cost‐efficient approach for the fabrication of conductive polymer hydrogels, which has a broad application prospect in flexible energy storage electronic devices. [ABSTRACT FROM AUTHOR]