Layered double hydroxides (LDHs) materials are widely used in the cathodes of high-performance supercapacitors. However, current preparation methods suffer from issues such as high energy consumption, complex processes, and significant safety hazards. In this study, based on a mild biomineralization reaction route, flower-like nano-sheet structured cobalt-based LDHs (COH) cathode was successfully prepared. The COH cathode achieved an outstanding specific capacitance of 829.0 F g-¹ at a current density of 1 A g-¹ and retained 90.9% of its initial capacitance after 4000 cycles. This biomineralization strategy holds promise for widespread application in the preparation of nanostructured electrode materials.