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The low‐cost processing and uniquely structured design of conducting polymer hydrogels (CPHs), with the advantages of both conducting polymers and 3D frameworks, are the keys to their wide commercial application in next‐generation flexible solid supercapacitors. Herein, an all‐sprayable hierarchically nanostructured polyaniline–phytic acid conducting polymer hydrogel (pp‐CPHs) for upgradable art patterns and massively manufactured supercapacitor electrodes is presented. Ascribing to fully anticipating the efficient electrode–electrolyte interface of 3D porous nanostructures constructed by interconnected nanorods, the pp‐CPH‐based flexible all‐solid‐state supercapacitors exhibit an excellent areal capacitance of 91 mF cm−2 at a current density of 1 mA cm−2 and a drastically improved cycling stability with 93.5% capacitance retention after 10 000 cycles at 5 mA cm−2. In addition, the electrochemical performance of this device can be constantly maintained under various mechanical loadings such as bending and twisting. Also, this device shows a remarkable integration ability from its universal tandem and parallel connections. Unambiguously, these aforementioned merits of pp‐CPH‐based flexible all‐solid‐state supercapacitors make it an ideal maneuver for the massive fabrication of flexible power supply. [ABSTRACT FROM AUTHOR]

Abstract Conducting polymer hydrogels (CPHs) advantageously synergize the features of both hydrogels and conducting polymers and have gained ground in various applications such as energy storage devices, catalysis and sensors. Conventional synthesis of CPHs usually couples with introducing of non-conductive polymer frameworks or chemical oxidative initiators, which will inevitably lead to degraded electrochemical performance and long rinse time. Here, we report an electrochemical polymerization method free of frameworks and initiators to build three-dimensional (3D) polyaniline/phytic acid supramolecular hydrogel. This CPH provides high conductivity of 0.43 S cm−1 and improved electrode interfaces between electronic transporting phase and ionic transporting phase. As a result, the CPHs exhibit large areal capacitance of 561.6 mF cm−2 and specific capacitance of 311.3 F g−1. Flexible solid-state micro-supercapacitors (MSCs) based on this CPHs deliver high areal capacitance of 135.9 mF cm−2 and considerable integratable potential via tandem and parallel connection. Cyclic stability is demonstrated by 10,000 galvanostatic charge/discharge cycles with 76% capacitance retention. Besides, electrochemical performance of this device can be maintained under different mechanical loadings such as bending and twisting, which makes it a promising power supply candidate for future wearable electronics and on-chip integrated circuit. Graphical abstract Image 1 [ABSTRACT FROM AUTHOR]