Utilizing alternative energy sources to fossil fuels has remained a significant issue for humanity. In this context, efficient earth-abundant bifunctional catalysts for water splitting and energy storage technologies like hybrid supercapacitors have become essential for achieving a sustainable future. Herein, CoCr-LDH@VNiS 2 was synthesized by hydrothermal synthesis. The CoCr-LDH@VNiS 2 catalyst entails 1.62 V cell voltage to reach the current density of 10 mA cm −2 for overall water splitting. The CoCr-LDH@VNiS 2 electrode illustrates a high electrochemical specific capacitance (Csp) of 1380.9 F g −1 at a current density of 0.2 A g −1 and an outstanding stability with 94.76% retention. Moreover, the flexible asymmetric supercapacitor (ASC) achieved an energy density of 96.03 W h kg −1 @0.2 A g −1 at a power density of 539.98 W kg −1 with remarkable cyclic stability. The findings provide a new approach toward the rational design and synthesis of bifunctional catalysts for water splitting and energy storage.

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