LAUSR

Controllably tailoring alloying anode materials to achieve fast charging and enhanced structural stability is crucial for sodium‐ion batteries with high rate and high capacity performance, yet remains a significant challenge owing to the huge volume change and sluggish sodiation kinetics. Here, a chemical tailoring tool is proposed and developed by atomically dispersing high‐capacity Ge metal into the rigid and conductive sulfide framework for controllable reconstruction of GeS bonds to synergistically realize high capacity and high rate performance for sodium storage. The integrated GeTiS3 material with stable Ti–S framework and weak GeS bonding delivers high specific capacities of 678 mA h g−1 at 0.3 C over 100 cycles and 209 mA h g−1 at 32 C over 10 000 cycles, outperforming most of the reported alloying type anode materials for sodium storage. Interestingly, in situ Raman, X‐ray diffraction (XRD), and ex situ transmission electron microscopy (TEM) characterizations reveal the formation of well‐dispersed NaxGe confined in the rigid Ti–S matrix with suppressed volume change after discharge. The synergistically coupled alloying‐conversion and surface‐dominated redox reactions with enhanced capacitive contribution and high reaction reversibility by a binding‐energy‐driven atomic scissors method would break new ground on designing a high‐rate and high‐capacity sodium‐ion batteries.