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Flexible graphene‐based paper electrodes (FGPEs) are a new class of study and the research on this electrode material has been carried out for approximately ten years. FGPEs have many advantages compared to classical solid electrodes such as being flexible, foldable, adaptable to flexible electronics, being cut, easily shaped, and effective and adjustable modification. In this work, the applicability of FGPEs modified with polyindole (PIN) thin films and zinc oxide nanoparticles (ZnO‐NPs) to energy‐storage systems as a supercapattery design is presented, and especially the limitations of ZnO‐NPs for energy‐storage applications are revealed to inform researchers working for a similar purpose. Capacitance calculations have been performed using both cyclic voltammetry (CV) and galvanostatic charge‐discharge (GCD) experiments. It was observed that the rGO/PIN paper demonstrated almost 30 times more energy‐storage capacity than that of the rGO/PIN/ZnO paper due to the electrochemical instability of ZnO‐NPs on the flexible electrode platform at the applied potential region in 1.0 M HClO4 solution. The rGO/PIN paper with a highly flexible property exhibited an energy density of 74.5 W h cm−2 and a power density of 2258 W cm−2 at a current density of 2.2 mA cm−2, revealing hopeful results for future modular and flexible approaches. [ABSTRACT FROM AUTHOR]

The flexible electrodes are the crucial components for fabricating wearable supercapacitors. In this study, we present a quick and convenient method to prepare graphene paper (GP) as a flexible current collector on a large scale by an easy one‐step method. The composite electrode integrated with GP and MnO2 as a flexible supercapacitor was obtained by an electrochemical deposition method without using binder or conductive agent. The substrate (GP) of electrode not only provides mechanical strength, but also contributes energy storage capacity. The MnO2 nanoparticles deposited on the surface of GP further improved the electrochemical performance of composite. The neat GP can give a specific capacitance of 184 F/g at a current density of 1 A/g. At a current density of 1 A/g, the specific capacitance of the GP/MnO2 composite with a deposition time of 30 s is as high as 410 F/g. The method presented here shows great potential for the development of flexible electrode materials in practical energy storage devices. [ABSTRACT FROM AUTHOR]