Lithium-rich layered oxide (LLO) are considered high-capacity cathode materials for next-generation lithium-ion batteries. In this study, LLO cathode materials were synthesized via the hydroxide coprecipitation method followed by a two-step lithiation process using different lithium contents and lithium sources. The effects of lithium content and lithium source on structure and electrochemical performance were investigated. This study demonstrated the clear impact of Li/TM ratio on electrochemical performance. Lower Li/TM ratio reduced the irreversible capacity loss in the first cycle and provided better cycling stability among all samples. The best results exhibited an initial discharge capacity of 279.65 mAh g−1 and reached a discharge capacity of 231.9 mAh g−1 (82.9% capacity retention) after 30 cycles. The sample using Li2CO3 as lithium source exhibits better electrochemical performance than the sample using LiOH as lithium source. Therefore, it is important to choose the appropriate lithium source and optimal lithium content for improving structural properties and electrochemical performance of LLO.