Nickel-cobalt (NiCo)-based materials have emerged as promising electrode candidates for advanced supercapacitors (SCs) owing to their multiple valence states, abundant redox-active sites, and tunable structural characteristics. However, their practical deployment is still constrained by challenges including limited electrical conductivity, structural instability during repeated redox cycling, and inefficient ion/electron transport, depending on their composition and electrode architecture. To address these limitations, recent research has increasingly focused on multidimensional structural and compositional engineering. This review systematically summarizes recent advancements in NiCo-based electrodes, including morphology control, self-supporting electrode construction, MOF-assisted derivatization, and functional coating strategies. Specifically, precise morphology control through synthetic parameters, ligand, and template regulation can increase active-site accessibility and facilitate ion transport. Integrating tailored NiCo-based structures onto conductive substrates to form binder-free, self-supporting electrodes reduces interfacial resistance and provides robust electrode architectures. In addition, MOFs serve as versatile structural platforms and precursors for deriving NiCo-based oxides, sulfides, phosphides, and layered double hydroxides (LDHs), which can improve electrical conductivity and structural stability while retaining favorable porous features. Furthermore, integrating NiCo-based materials with functional components such as carbon materials, MXenes, and transition-metal compounds provides additional opportunities to regulate interfacial charge transfer and structural stability through multicomponent interactions. Finally, this review discusses current challenges and future perspectives, including interfacial evolution revealed by in-situ/operando characterization, rational material design assisted by theoretical calculations and machine learning, and the practical development of high-performance NiCo-based supercapacitor electrodes.



