Nanostructure engineering and composition rationalization are crucial for materials to become candidates for high-performance supercapacitor. Herein, a novel core-shell heterostructured electrode, combining CoS hollow nanorods with NiCoMn-layered double hydroxides (LDH) ternary metal nanosheets, were prepared on carbon cloth by reasonably controlled vulcanization and electrodeposition. By optimizing electrodeposition conditions, the material's structure and properties can be fine-tuned. The enhanced capacitance of the optimized carbon cloth (CC)@CoS/NiCoMn-LDH-300 electrode (4256.0 F g−1) lies in the open space provided by CoS and the establishment of a new charge transfer channel across the interfaces of CC@CoS/NiCoMn-LDH-300 nanosheets. This is further demonstrated by Density functional theory (DFT) simulations based on OH− adsorption energy, which produces faster redox charge kinetics and significantly enhances the electrode's energy storage capacity. The hybrid supercapacitor, integrating the optimized CC@CoS/NiCoMn-LDH-300 electrode with active carbon, demonstrates the highest energy density of 86 Wh kg−1 (under the power density of 850 W kg−1) and the long cycle stability of 89.7%. This study aims to go beyond simple binary LDH by constructing a ternary LDH with a hierarchical core-shell heterostructure to provide an effective and feasible new concept for high-performance supercapacitor electrode materials via rational structure design.
