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Spherical Li[Ni_0.8Co_0.2−xMn_x]O₂ (x=0, 0.1) with phase-pure and well-ordered layered structure have been synthesized by heat-treatment of spherical [Ni_0.8Co_0.2−xMn_x](OH)₂ and LiOH·H₂O precursors. The structure, morphology, electrochemical properties, and thermal stability of Li[Ni_0.8Co_0.2−xMn_x]O₂ (x=0, 0.1) were studied. The average particle size of the powders was about 10–15μm and the size distribution was narrow due to the homogeneity of the metal hydroxide [Ni_0.8Co_0.2−xMn_x](OH)₂ (x=0, 0.1). The Li[Ni_0.8Co_0.2−xMn_x]O₂ (x=0, 0.1) delivered a discharge capacity of 197–202mAhg⁻¹ and showed excellent cycling performance. Compared to Li[Ni_0.8Co_0.2]O₂, Li[Ni_0.8Co_0.1Mn_0.1]O₂ exhibited greater thermal stability resulting from improved structural stability due to Mn substitution.