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Chalcogenide cathodes with multi‐electron transfer characteristics are indispensable to aluminum‐ion batteries (AIBs). Nevertheless, their grievous capacity degradation and sluggish reaction kinetics remain fundamental challenges for the practical application. Herein, a Cu2S/Ni3S2 multiphase structure within the metal‐organic frame (MOF) derived carbon decoration layer (CNS@MC) is constructed to elevate the intrinsic electronic properties of chalcogenide cathode and realize high‐performance AIBs. The existence of outer carbon layer and strong orbital interaction at inner heterointerfaces eliminates the bandgap and arises more electrons at Fermi level, efficiently reducing the energy barrier for electron transfer and achieving high reactivity within cathodes. The CNS@MC also presents a strong electronic interaction with active solvent groups, which is beneficial to capture Al3+ and facilitate the three‐electron charge‐storage reactions. Experimental results demonstrate that the tailored CNS@MC cathode possesses superior redox kinetics due to the sufficient surface area and rapid Al‐ion diffusion during cycling. Meanwhile, the robust CNS@MC delivers ultra‐high electrochemical stability (131.1 mAh g−1 over 3500 cycles) with high coulombic efficiency and outstanding rate performance. This work offers new opportunities for optimizing the intrinsic properties of the chalcogenide electrodes based on MOF derivatives and heterostructure, providing novel thoughts for designing high‐performance AIBs. [ABSTRACT FROM AUTHOR]

Aqueous static zinc–iodine batteries attract tremendous attention because of their abundant reserves of iodine, nonflammable electrolyte, and facile assembly. Currently, scientific challenges for static zinc–iodine batteries include self‐discharge and sluggish kinetics. Herein, a lithiation approach for the iodine host to suppress the shuttle effect and catalyze iodine conversion is reported. Through regulating the d‐ and p‐band center and lowering the I−/I0 conversion barrier, Li+ intercalation into VS2 reinforces interaction with I3− and achieves catalytic conversion of iodine, ameliorating self‐discharge, and accelerating kinetics. Zinc–iodine batteries featuring LiVS2 as the iodine host reach a high iodine utilization, high Coulombic efficiencies, and a long cyclic lifespan. Notably, the performance enhancement mechanism is the thermodynamically favorable iodine conversion reaction, inhibition of the I3− appearance, and promotion of I3− consumption due to the Li+ insertion. The findings provide fundamental insights into tackling issues of static zinc–iodine batteries. [ABSTRACT FROM AUTHOR]