Rational morphology design and size control have been demonstrated an effective strategy to improve the electrochemical performance of cathode materials for lithium ion batteries. In this work, different morphologic Li-rich layered cathode materials Li1.2Mn0.54Ni0.13Co0.13O2 with hierarchical structures are conveniently synthesized through a facile solvothermal route followed by calcination treatment. The morphology and size of the as-prepared precursors are easily regulated by changing the addition of organic solvent with different viscosity and polarity. And their critical impacts on the microstructure and electrochemical property of Li-rich layered electrodes are further systematically investigated. In particular, the hierarchical structured Li1.2Mn0.54Ni0.13Co0.13O2 microspheres exhibit superior electrochemical performance and excellent cycling stability among all samples, delivering a discharge capacity of 281.9 mAh g−1 at 0.1 C with 84.8% retention after 100 cycles. A high discharge capacity of 143.0 mAh g−1 still can be achieved even at a high current density of 5 C. Besides, this work would also provide an effective and feasible strategy for the morphology controllable synthesis of high energy density oxide electrode materials for lithium ion batteries.