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Layered transition metal dichalcogenides have great potential as anodes of sodium‐ion batteries (SIBs) due to their high theoretical specific capacity. However, the restacking severely limits their accessible sites, leading to undesirable specific capacity, cycle stability, and working temperature range. Herein, a hierarchical 2D VS2/Ti3C2Tx MXene hybrid is designed via a simple liquid‐mixing method, where VS2 is confined in the conductive Ti3C2Tx matrix with chemical connections built between them. The in situ transmission electron microscopy analyses reveal that the hybrid depends on a very fast and reversible intercalation/de‐intercalation process between VS2 and NaxVS2 (where x = 1) to store sodium. Theoretical calculations disclose that the Ti3C2Tx matrix remarkably enhances the charge transfer and alleviates the volume expansion of VS2 especially after Na+ is inserted. Consequently, such a rational design exhibits an intercalation pseudocapacitance‐dominant mechanism, with excellent specific capacity (522 mAh g−1 at 0.2 A g−1), rate capability (342 mAh g−1 at 10 A g−1), cycle life (116% after 3000 cycles), and also all‐climate workability (with high specific capacity and long‐term cycle stability even at 70 and −40 °C). This study may open up a new vision to design fast‐charging, long‐cycle, and all‐climate SIBs anodes based on the intercalation pseudocapacitance. [ABSTRACT FROM AUTHOR]

Metals fluorides (MFs) are potential conversion cathodes to replace commercial intercalation cathodes. However, the application of MFs is impeded by their poor electronic/ionic conductivity and severe decomposition of electrolyte. Here, a composite cathode of FeF2 and polymer‐derived carbon (FeF2@PDC) with excellent cycling performance is reported. The composite cathode is composed of nanorod‐shaped FeF2 embedded in PDC matrix with excellent mechanical strength and electronic/ionic conductivity. The FeF2@PDC enables a reversible capacity of 500 mAh g–1 with a record long cycle lifetime of 1900 cycles. Remarkably, the FeF2@PDC can be cycled at a record rate of 60 C with a reversible capacity of 107 mAh g–1 after 500 cycles. Advanced electron microscopy reveals that the in situ formation of stable Fe3O4 layers on the surface of FeF2 prevents the electrolyte decomposition and leaching of iron (Fe), thus enhancing the cyclability. The results provide a new understanding to FeF2 electrochemistry, and a strategy to radically improve the electrochemical performance of FeF2 cathode for lithium‐ion battery applications. [ABSTRACT FROM AUTHOR]