为了促进高端便携式电子产品进一步发展，迫切需要发展具有高能量密度和高功率密度特性（简称“双高”）的锂离子电池（LIBs）。钴酸锂（LiCoO₂）是目前商业化最为成功的正极材料，却仍然面临着工作电压较低和快充能力不足的挑战，远未达到双高储能目标的要求。在此，我们系统地总结和讨论了高电压和快充钴酸锂正极的研究现状，深入探讨了该领域的关键基础挑战、多种改性策略的最新研究进展和未来展望。本文首先全面详细地讨论了钴酸锂关键失效机制，包括体相结构退化、界面结构失稳、非均质反应过程和缓慢的界面反应动力学。随后，文中对已发展的改性策略和改性机制进行了归纳总结，分为通过元素掺杂（包括锂位点、钴位点、氧位点和多位点掺杂）提升锂离子扩散速率和体相结构稳定性以及通过表面包覆（包括电介质、离子导体、电子导体材料及其组合）提升表界面结构稳定性和离子/电子导电性、纳米化、多策略组合及其他策略（包括电解质、黏合剂、电极的曲折度、充电协议和预锂化方法的优化）。最后，我们对前瞻性观点和具有前景的研究方向进行了深入阐述，为设计和实现用于下一代双高锂离子电池的高电压快充钴酸锂正极提供了独到的建议和理论指导。

Lithium-ion batteries (LIBs) with the “double-high” characteristics of high energy density and high power density are in urgent demand for facilitating the development of advanced portable electronics. However, the lithium ion (Li⁺)-storage performance of the most commercialized lithium cobalt oxide (LiCoO₂, LCO) cathodes is still far from satisfactory in terms of high-voltage and fast-charging capabilities for reaching the double-high target. Herein, we systematically summarize and discuss high-voltage and fast-charging LCO cathodes, covering in depth the key fundamental challenges, latest advancements in modification strategies, and future perspectives in this field. Comprehensive and elaborated discussions are first presented on key fundamental challenges related to structural degradation, interfacial instability, the inhomogeneity reactions, and sluggish interfacial kinetics. We provide an instructive summary of deep insights into promising modification strategies and underlying mechanisms, categorized into element doping (Li-site, cobalt-/oxygen-site, and multi-site doping) for improved Li⁺ diffusivity and bulk-structure stability; surface coating (dielectrics, ionic/electronic conductors, and their combination) for surface stability and conductivity; nanosizing; combinations of these strategies; and other strategies (i.e., optimization of the electrolyte, binder, tortuosity of electrodes, charging protocols, and pre-lithiation methods). Finally, forward-looking perspectives and promising directions are sketched out and insightfully elucidated, providing constructive suggestions and instructions for designing and realizing high-voltage and fast-charging LCO cathodes for next-generation double-high LIBs.