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To drive electrical vehicles for long‐range, the energy density of Li‐ion batteries must be further enhanced, which requires high‐energy cathode materials. Among them, Ni‐rich LiNixMnyCo1−x–yO2 (x > 0.5, NMC) is one of the most promising candidates. However, traditional poly‐crystal (PC) NMC materials, whose particles are secondary clusters consisting of many primary crystalline particles, are susceptible to pulverization along the inter grain/particle boundaries, resulting in poor cycle stability. Recently, single crystal (SC)‐NMC cathodes are proposed as they are believed to have several merits such as high structural integrity, lower interface with electrolyte, and potentially better energy storage performance. Nevertheless, several queries, such as the merits of SC structure and the mechanism for their structure degradation, are still controversial and required to be addressed. Herein, the synthesis parameters, properties, energy storage as well as safety of SC‐ and PC‐NMC cathodes with various Ni contents are critically reviewed, for clarifying the merits and drawbacks of SC. Furthermore, the study focuses on the recent advances of insight mechanisms and strategies for stabilizing the structure/interface by doping, morphology engineering, surface coating, and composition tailoring. The remaining challenges, safety concerns, and perspectives to enhance the electrochemical performance of SC‐NMC cathodes for electric vehicle application are followed. [ABSTRACT FROM AUTHOR]