The layered Ni-rich NiCoMn (NCM)-based cathode active material Li[NixCo(1-x)/2Mn(1-x)/2]O2 (x ≥ 0.6) has the advantages of high energy density and price competitiveness over an LiCoO2-based material. Additionally, NCM is beneficial in terms of its increasing reversible discharge capacity with the increase in Ni content; however, stable electrochemical performance has not been readily achieved because of the cation mixing that occurs during its synthesis. In this study, various layer-structured Li1.0[Ni0.8Co0.1Mn0.1]O2 materials were synthesized, and their electrochemical performances were investigated. A NiCoMnCO3 precursor, prepared using carbonate co-precipitation with Li2CO3 as the lithium source and having a sintering temperature of 850 °C, sintering time of 25 h, and metal to Li molar ratio of 1.00–1.05 were found to be the optimal parameters/conditions for the preparation of Li1.0[Ni0.8Co0.1Mn0.1]O2. The material exhibited a discharge capacity of 160 mAhg−1 and capacity recovery rate of 95.56% (from a 5.0–0.1 C-rate).