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Li-rich layered oxides have aroused much interest in high-energy cathode materials for Li-ion batteries (LIBs). However, they still come with significant challenges of appreciable voltage decay and hysteresis upon cycling. Microstructure and surface are considered to be crucial for the stabilization of high-capacity Li-rich layered oxide cathode. In this work, we report the controlled synthesis of unique Li-rich layered nanobelts through nanolayer-confined crystal growth. The unique one-dimensional Li1.2Mn0.54Co0.13Ni0.13AlxO2 nanostructures and reconstruction of spinel phase domains may not only offer fast Li-ion diffusion pathways, but inhibit the structural collapse and mitigate the voltage decay upon discharge/charge cycling. The cathode made of Li1.2Mn0.54Co0.13Ni0.13AlxO2 layered/spinel nanobelts exhibits enhanced rate capability and long-term cyclability. An initial discharge capacity of 283.5 mA h g−1 at 0.1 C and the capacity retention of 88.1% over 100 cycles at 1 C are achieved. This work may pave an avenue toward nanostructuring and surface engineering of electrode materials and practical applications of high-energy-density LIBs.