Multiscale Regulation of Metal–Organic Frameworks in Lithium‐Ion Battery Separators: Mechanism, Strategy, and Performance Optimization

Lithium‐ion polypropylene (PP) separators limit high‐energy Li‐ion batteries due to poor thermal stability, low wettability, and weak dendrite suppression. Metal–organic frameworks (MOFs) provide a viable solution through tunable pores, high surface area, and versatile surface chemistry. This review summarizes multiscale regulation strategies for MOFs‐modified PP separators. It classifies applicable MOFs into three topological types—ZIF, UiO, and HKUST—and analyzes their distinct mechanisms in enhancing ion transport and interfacial dynamics. Four primary fabrication techniques (coating, blending, in situ growth, and composite construction) are systematically compared for their suitability and performance outcomes. Key challenges remain, including high costs, poor interface compatibility, and insufficient long‐term stability. Future development requires integrating multiscale structural engineering, intelligent dynamic interfaces, and cost‐effective green manufacturing. This review offers a practical framework for designing advanced separators for next‐generation high‐safety, high‐energy‐density Li‐ion batteries.