A 3D Heterostructural Composite Comprising MOF‐Derived Ni(OH)2 and NiAl LDH on rGO for Supercapacitors

Comprehensive Summary The development of high‐performance cathode materials through rational heterointerface engineering remains pivotal for advancing hybrid supercapacitors (HSCs) technologies. Here, we construct a three‐dimensional ternary heterostructure composite Ni(OH) 2 /NiAl LDH/rGO (N‐OH/NA/rG) by sequential integration of metal‐organic frameworks (MOF)‐derived Ni(OH) 2 , NiAl LDH and reduced graphene oxide (rGO). The covalent anchoring of NiAl LDH nanosheets on oxygen‐functionalized rGO substrates mitigates restacking issues, establishing a conductive network with enhanced charge transfer kinetics. The alkaline etching of Ni‐MOF precursors preserves their hierarchical porosity while converting to pseudocapacitive Ni(OH)₂. Synergistic effects among components yield increased active site density, dual charge storage mechanisms, and optimized ion diffusion pathways. The optimized composite achieves a high specific capacitance of 1481.7 F/g at 1A/g, along with excellent rate capability and cycle performance, establishing a new paradigm for designing multi‐component heterostructure electrodes through MOF‐derived interface engineering. Furthermore, the N‐OH/NA/rG//AC HSC device demonstrates a high power density and energy density, coupled with long‐term cycle stability, underscoring the substantial potential of N‐OH/NA/rG as a cathode material for HSCs.