For conventional polycrystalline Ni‐rich cathode material consisting of numerous primary particles in disordered orientation, the crystal anisotropy in charge/discharge process results in the poor rate capability and rapid capacity degradation. In this work, highly‐dispersed submicron single‐crystal LiNi0.8Co0.15Al0.05O2 (SC‐NCA) cathode is efficiently prepared by spray pyrolysis (SP) technique followed by a simple solid‐state lithiation reaction. Porous Ni0.8Co0.15Al0.05Ox precursor prepared via SP exhibits high chemical activity for lithiation reaction, enabling the fabrication of single‐crystal cathode at a relatively low temperature. In this way, the contradiction between high crystallinity and cation disordering is well balanced. The resulted optimized SC‐NCA shows polyhedral single‐crystal morphology with moderate grain size (≈1 μm), which are beneficial to shortening the Li+ diffusion path and improving the structural stability. As cathode for lithium ion batteries, SC‐NCA delivers a high discharge capacity of 202 and 140 mAh g−1 at 0.1 and 10 C, respectively, and maintains superior capacity retention of 161 mAh g−1 after 200 cycles at 1C. No micro‐crack is observed in the cycled SC‐NCA particles, indicating such single‐crystal morphology can greatly relieve the anisotropic micro‐strain. This effective, continuous and adaptable strategy for preparing single‐crystal Ni‐rich cathode without any additive may accelerate their practical application.

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Single-crystal nickel-rich cathode materials (SC-NRCMs) are the most promising candidates for next-generation power batteries which enable longer driving range and reliable safety. In this review, the outstanding advantages of SC-NRCMs are discussed systematically in aspects of structural and thermal stabilities. Particularly, the intergranular-crack-free morphology exhibits superior cycling performance and negligible parasitic reactions even under severe conditions. Besides, various synthetic methods are summarized and the relation between precursor, sintering process, and final single-crystal products are revealed, providing a full view of synthetic methods. Then, challenges of SC-NRCMs in fields of kinetics of lithium diffusion and the one particularly occurred at high voltage (intragranular cracks and aggravated parasitic reactions) are discussed. The corresponding mechanism and modifications are also referred. Through this review, it is aimed to highlight the magical morphology of SC-NRCMs for application perspective and provide a reference for following researchers.