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Integrated spinel-layered cathode materials are much appeal for use in high-energy-density Li-ion batteries. Here, we introduce a one-step hydrothermal reaction to synthesize high-capacity cathode materials (>300 mAh g−1) based on Li–Mn–O systems. The synthesis temperature governs the phase components and cation disorder. The sample with a low synthesis temperature (150 °C) shows the highest capacity (320 mA h g−1, 2–4.8 V) but the capacity decreases intensely to 62% after 50 cycles. The sample with the higher synthesis temperature (200 °C) shows better cycling stability with 85% capacity retention after 50 cycles. This study elucidates the roles of cation disorder as well as the spinel phase on the high-capacity cathode and provides an understanding of their electrochemical behaviors.