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The lithium-rich layered oxides are one of the most attractive cathode materials for lithium-ion batteries. Here, two types of Li1.20Ni0.32Co0.004 Mn0.476O2 were synthesized using Li2CO3 and LiOH as lithium sources. An electrochemical activation process occurs in Li1.2Ni0.32Co0.004 Mn0.476O2 prepared from Li2CO3 (LLO-1), while no obvious activation in Li1.2Ni0.32Co0.004Mn0.476O2 prepared from LiOH (LLO-2) is observed. Via advanced scanning transmission electron microscopy (STEM), we found that Li2MnO3-like structure is rich in the surface region of LLO-2. The study provides a direct explanation for the electrochemical activation of lithium-rich materials. The sample with more LiMO2-like phase at the surface region shows a better cycling performance. It is likely that more LiMO2-like phase at the surface region could stabilize the interface and improve the cycling performance of the Li-rich cathode materials.