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Summary In this study, we followed a facile method to grow well‐aligned PANI nanostructures on S‐doped reduced graphene oxide nanosheets (SPANI/S‐rGO) using hydrothermal method combined with soft template polymerization of aniline where naphthalene sulfonic acid is used as a dopant for PANI as well as the soft template. The effect of using different wt% of S‐rGO on the structural, morphology, and electrochemical performance of SPANI/S‐rGO composites has been evaluated. Supercapacitor fabricated using SPANI/S‐rGO10 (10 wt% of S‐rGO) composite based electrodes delivered a high specific capacitance of 347.5 F/g at a current density of 1 A/g in symmetrical cell design (the specific capacitance was calculated based on a single electrode). Only 11% of its initial capacitance is lost after 2500 cycles at a current density of 2 A/g. The enhanced performance is attributed to the optimum loading of S‐rGO in designing binary composite, well‐aligned growth of SPANI nanostructures on S‐rGO sheets, and synergistic effect of both S‐rGO and SPANI. The facile synthesized SPANI/S‐rGO composite electrode material with the aforementioned features is considered to be a promising candidate for a high‐performance supercapacitor.

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2D multilayered reduced graphene oxide (rGO) has received enormous research interest as a potential electrode material for flexible supercapacitor (FSC), owing to its excellent electrochemical and mechanical properties. However, rGO suffers from the restacking of graphene (GN) layers, lower electrical conductivity resulting from the residual oxygen functional groups and the relatively poor real-time electrochemical performance. One of the finest ways overcoming the drawbacks of rGO by doping heteroatom into GN network and surface modification to enhance its electrochemical properties. In this work, a simple and robust approach for designing an efficient and high-performance flexible electrode with nitrogen-doped reduced graphene oxide (N-rGO) framework coupled with surface modification through in situ chemical polymerization with aniline to form a long-range interconnected polyaniline (PANI) nanostructure is presented. In a two-electrode system, PANI/N-rGO flexible electrode has delivered a higher specific capacitance of 322 F g À1 at a current density of 1 A g À1 . Further, the composite exhibited notable cyclic stability over 1000 charge-discharge cycles. Surface-modified in-situ grown PANI nanostructures on N-rGO nanosheets prevent the volume changes that occur in PANI during the charge-discharge process, and offer a higher charge transportation rate throughout the surface area. As a result of enhanced electrochemical properties, PANI/N-rGO composites provide a feasible route for designing FSCs.