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Engineering interfacial properties of metal‐sulfides toward excellent electrochemical capability is imperative for advanced energy‐storage materials. However, they still suffer from an unclear mechanism of capacity fading, along with ineffective physical–chemical evolution. Herein, a highly‐effective Sb₂S₃ with double carbon is designed with interfacial SbC bonds and double carbon, which boosts promoting of ion transferring and alleviates the separation of both active phases (Sb, S). Through “voltage‐cutting” manners, the key elements of capacity improvement about phase transitions are further determined. As expected, even at 5.0 A g⁻¹, the lithium‐storage capacity remains about 674 mAh g⁻¹. Utilized as sodium ion battery (SIB) anode, the rate capacity still reaches up to 366 mAh g⁻¹ at 3.0 A g⁻¹, much larger than that of Sb₂S₃. Obtaining the full cell of Ni–Fe Prussian blue analog versus M‐Sb₂S₃@DC …