Aqueous zinc-ion batteries (AZIBs) are promising for large-scale energy storage systems due to their high safety, large capacity, cost-effectiveness, and environmental friendliness. However, their commercialization is currently hindered by several challenging issues, including cathode degradation and zinc dendrite growth. Recently, metal-organic frameworks (MOFs) and their derivatives have gained significant attention and are widely used in AZIBs due to their highly porous structures, large specific surface area, and ability to design frameworks for Zn²⁺ shuttle. Based on preceding contributions, this review aims to generalize two design principles for MOF-based materials in AZIBs: cathode preparation and anode protection. For cathode preparation, we mainly introduce novel MOF-based electrode materials such as pure MOFs, porous carbon materials, metal oxides, and their compounds, focusing on the analysis of the specific capacity of AZIBs. For anode protection, we systematically analyze MOF-based materials used as 3D Zn architecture, solid electrolyte interfaces, novel separators, and solid-state electrolytes, highlighting the improvement in the cyclic stability of Zn anodes. Finally, we propose the future development of MOF-based materials in AZIBs. Our work can give some clues for raising the practical application level of aqueous ZIBs.

Lithium (Li) dendrite formation and poor Li⁺ transport kinetics under high‐charging current densities and capacities inhibit the capabilities of Li metal batteries (LMBs). This study proposes a 3D conductive multichannel carbon framework (MCF) with homogeneously distributed vertical graphene nanowalls (VGWs@MCF) as a multifunctional host to efficiently regulate Li deposition and accelerate Li⁺ transport. A novel electrode for both Li|VGWs@MCF anode and LFP|VGWs@MCF (NCM₈₁₁|VGWs@MCF) cathode is designed and fabricated using a dual vertically aligned architecture. This unique hierarchical structure provides ultrafast, continuous, and smooth electron transport channels; furthermore, it furnishes outstanding mechanical strength to support massive Li deposition at ultrahigh rates. As a result, the Li|VGWs@MCF anode exhibits outstanding cycling stability at ultrahigh currents and capacities (1000 h at 10 mA cm^–2 and 10 mAh cm^–2, and 1000 h at 30 mA cm^–2 and 60 mAh cm^–2). Moreover, full cells made of such 3D anodes and freestanding LFP|VGWs@MCF (NCM₈₁₁|VGWs@MCF) cathodes with conspicuous mass loading (45 mg cm^–2 for LFP and 35 mg cm^–2 for NCM₈₁₁) demonstrate excellent areal capacities (6.98 mAh cm^–2 for LFP and 5.6 mAh cm^–2 for NCM₈₁₁). This strategy proposes a promising direction for the development of high‐energy‐density practical Li batteries that combine safety, performance, and sustainability.