Abstract: Ni-rich layered material is a kind of high-capacity cathode to meet the requirement of electric vehicles. As for the typical LiNi_0.8Co_0.1Mn_0.1O₂ material, the particle formation is significant for electrochemical properties of the cathode. In this work, the structure, morphology, and electrochemical performance of LiNi_0.8Co_0.1Mn_0.1O₂ secondary particles and single crystals were systematically studied. A lower Ni²⁺/Ni³⁺ molar ratio of 0.66 and a lower residual alkali content of 0.228wt% were achieved on the surface of the single crystals. In addition, the single crystals showed a discharge capacity of 191.6 mAh/g at 0.2 C (~12 mAh/g lower than that of the secondary particles) and enhanced the electrochemical stability, especially when cycled at 50°C and in a wider electrochemical window (between 3.0 and 4.4 V vs. Li⁺/Li). The LiNi_0.8Co_0.1Mn_0.1O₂ secondary particles were suitable for applications requiring high specific capacity, whereas single crystals exhibited better stability, indicating that they are more suitable for use in long life requested devices.