Microscopic Insight of the High‐Entropy Effect on the Lithium Storage Performance and Rate Capability of Spinel Oxide

High‐entropy spinel oxides are promising anode materials for lithium‐ion batteries owing to their unique crystal structures, which provide enhanced structural stability, multiple redox‐active sites, and three‐dimensional Li⁺ diffusion pathways. However, the intrinsic complexity and compositional diversity of high‐entropy systems have limited a comprehensive understanding of the correlation between crystal structure, elemental composition, and rate performance, thereby impeding further optimization and practical application. In this study, a high‐entropy spinel oxide (Fe_0.2Co_0.2Ni_0.2Cr_0.2Zn_0.2)₃O₄ (FCNCZO) is synthesized to investigate its electrochemical properties. The material delivers a high reversible capacity of 551 mAh g⁻¹ at 500 mA g⁻¹ after 110 cycles and maintains an excellent rate capability of 330 mAh g⁻¹ at a high current density of 2000 mA g⁻¹. Density functional theory calculations indicate that the synergistic interaction among multiple metal elements reduces the bandgap and broadens the d‐band width. Moreover, the high‐entropy effect promotes metal‐oxygen orbital hybridization, facilitates charge redistribution, and significantly enhances rate capability. These findings provide new microscopic insights into the high‐entropy effect and demonstrate its potential in designing next‐generation high‐entropy anode materials with superior rate performance for high‐power lithium‐ion batteries.