0.5Li2MnO3·0.5LiMn1/3Ni1/3Co1/3O2 microspheres are prepared by a slurry spray-drying process (SD-LLO) with subsequent heat treatment. SEM images show that the SD-LLO microspheres are composed of nano-size primary particles. These particles are quite different from conventional LLO microspheres, which are composed of micron-scale plate-like primary particles prepared by a co-precipitation method (CP-LLO). The SD-LLO material experiences a smaller voltage drop during cycling than CP-LLO when used as cathode material in lithium-ion batteries. High-resolution transmission electron microscopy (HR-TEM) and energy dispersive spectroscopy (EDS) indicate that the smaller voltage drop of SD-LLO can be attributed to a more homogeneous distribution of transition metals.