LAUSR

The development of fast‐charging lithium‐ion batteries requires electrode materials with both high‐rate capability and excellent durability. Here an entropy‐tuned niobium‐based oxide (ETNO) anode is introduced, strategically engineered through multi‐cation doping by incorporating Nb5+, Ti4+, W6+, Fe3+, and Ca2+ into the Wadsley‐Roth shear structure of niobium oxide. ETNO demonstrates high‐rate capability, delivering 171 mAh g−1 at 20.0 A g−1, and retains 79% of its initial capacity after 9,000 cycles under extreme fast‐charging conditions. X‐ray diffraction (XRD) and operando Raman spectroscopy reveal that the entropy tuning enables a gradual structural transformation during (de)lithiation, facilitating stable phase evolution and minimizing strain. Computational analysis confirms that entropy tuning enhances Li‐ion diffusion, reduces bandgap energy, and mitigates volume expansion, collectively improving electrochemical performance. Full cell testing with a LiNi0.8Mn0.1Co0.1O2 (NMC811) cathode validates the practical viability of ETNO, demonstrating superior cycling stability and high capacity retention. This study establishes entropy tuning as a powerful design strategy for next‐generation high‐power lithium‐ion battery anodes, offering exceptional fast‐charging capability and durability.