Li-rich layered oxide materials possess high voltage and high specific capacity, which makes them attractive cathode candidates for lithium-ion batteries. However, they still suffer from a poor rate capability, which seriously blocks their widespread practical applications. In this work, Li(Li0.167Mn0.5Co0.167Ni0.167)O2 microspheres were synthesized by a hydrothermal-assisted method, in which Ni-Co-Mn-based microspherical precursors obtained by a hydrothermal process with polyethylene glycol-600 (PEG-600) as a surfactant were mixed with lithium sources and then sintered to yield the final products. It is found that the as-prepared Li-rich layered oxide microspheres exhibit high discharge capacity and superior rate performance: delivering an initial discharge capacity of 292mAhg−1 at a current density of 20mAg−1, 189mAhg−1 at a current density of 600mAg−1 and 142mAhg−1 at a current density of 2000mAg−1 (10C), which are better than that of the sample as-prepared by co-precipitation method. The high discharge capacity and improved rate-capability were beneficial from the microspheres assembled by uniform primary particles around 250nm, more reversible redox and better electrode kinetics comparing to that of the co-precipitation sample. The preparation strategy reported here may offer hints for achieving various advanced Li-rich layered composite materials that would be used in high-performance energy storage.