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Ni‐rich layered oxide cathode material with Ni contents greater than 90% is considered as a highly promising candidate for lithium‐ion batteries (LIBs) owing to its remarkable specific capacity and cost‐efficiency. However, severe capacity degradation caused by the structural collapse and interfacial instability with electrolyte under high voltage greatly hinders the practical application. Here, an antimony (Sb)‐doped LiNi0.91Co0.06Al0.03O2 (Sb‐NCA91) cathode is proposed, where the Sb doping modifies the morphology of primary particles and enables the radially aligned microstructure. This unique microstructure can disperse the anisotropic mechanical stress caused by the H2‐H3 phase transformation, and mitigate the shrinkage and expansion of the primary particles during high‐voltage and low‐temperature cycling, thus inhibiting the formation of microcracks and structural deterioration. Meanwhile, the closely arranged radial spokes allow fast ion transport in the secondary particles and effectively improve the rate performance and low‐temperature performance of the cathodes. As a result, the Sb modified cathode demonstrates superior capacity retention of ≈84% at 1 C after 200 cycles in 2.7–4.5 V at 25 °C, while the pristine NCA91 cathode only retains ≈79%. Additionally, the capacity retention at −20 °C is significantly increased from ≈61% (NCA91) to ≈88% (Sb‐NCA91) after 100 cycles. [ABSTRACT FROM AUTHOR]