Spherically shaped 0.3Li 2 MnO 3 ·0.7LiNi 0.5 Mn 0.5 O 2 composite cathode powders with filled morphology and narrow size distribution are prepared by large-scale spray pyrolysis. A droplet classification reduces the standard deviation of the size distribution of the composite cathode powders. Addition of boric acid improves the morphological properties of the product powders by forming a lithium borate glass material with low melting temperature. The optimum amount of boric acid dissolved in the spray solution is 0.8wt% of the composite powders. The powders prepared from the spray solution with 0.8wt% boric acid have a mixed layered crystal structure comprising Li 2 MnO 3 and LiNi 0.5 Mn 0.5 O 2 phases, thus forming a composite compound. The initial charge and discharge capacities of the composite cathode powders prepared from the 0.8wt% boric acid spray solution are 297 and 217mAhg −1 , respectively. The discharge capacity of the powders decreases from 217 to 196mAhg −1 by the 30th cycle, in which the capacity retention is 90%.