Interface‐Orchestrated Dual Microenvironments in CDMOF/MXene for Selective Dye Adsorption and Lithium–Sulfur Battery Enhancement

Abstract With increasing environmental pollution and the global energy crisis, developing advanced materials that can selectively capture pollutants and efficiently convert energy is crucial. A dual microenvironment strategy featuring polar interfacial groups and a supramolecular recognition cavity is reported. The integrated design enables both efficient dye adsorption and high‐performance energy storage. Cyclodextrin‐based metal–organic frameworks (CDMOFs) are rapidly grown on MXene nanosheets via a microwave‐assisted in situ method, forming a spatially organized architecture with functional complementarity. This CDMOF/MXene shows high selectivity toward malachite green (MG), achieving a maximum adsorption capacity of 960.3 mg g −1 . The performance arises from host–guest recognition within cyclodextrin cavities and enhanced adsorption from polar MXene surfaces. In lithium–sulfur (Li–S) batteries, the polar surface groups on MXene work synergistically with the oxygen‐rich cavities of CDMOF. This collaboration establishes a multistep mechanism of “recognition–immobilization–conversion,” which effectively suppresses polysulfide shuttling. Density functional theory (DFT) calculations confirm the interfacial synergy between the dual microenvironments. As a result, the assembled Li–S batteries exhibit remarkable cycling stability over 1000 cycles. This work demonstrates a generalizable approach for constructing multifunctional materials through interfacial engineering, offering valuable insights into the integration of pollutant capture and energy storage.