Huili Zhao, Li Wang, S. Y. Li, Jiashuo Xie, Min Ji, Min Wang
High‐nickel cathodes attract increasing attention owing to their high specific capacity, yet exhibit structural instability and inferior cycling performance. Surface coating is an effective strategy to enhance their electrochemical behavior. This study introduces a nitrogen‐doped zirconia‐carbon composite (NC@ZrO 2 ) as a coating for LiNi 0.8 Mn 0.1 Co 0.1 O 2 (NCM811), with the composite prepared using the metal–organic framework material UiO‐66‐NH 2 as a precursor. As a coating layer, NC@ZrO 2 prevents direct contact between cathode and electrolyte to suppress side reactions and reduce interfacial resistance. Its porous structure facilitates lithium‐ion diffusion. Consequently, the modified NCM811 presents remarkable rate capability and cycling stability. The 10 wt% coated NCM811 cathode demonstrates 78.3% capacity retention at 5 C, exceeding that of the unmodified NCM811 by 36.4%. After 500 cycles at 1 C, the modified material retains 82.4% capacity retention. This work presents a promising approach for optimizing high‐nickel cathode materials using MOF‐based composites.