Layered Li1.2Mn0.54Ni0.13Co0.13O2 materials were synthesized via spray pyrolysis. Synthesis conditions were varied in order to understand their effect on the electrochemical properties of the material. Three process parameters were evaluated: aerosol flow rate, reactor wall temperature and precursor concentration. Electrochemical results show excellent batch-to-batch reproducibility and no non-uniformities, as measured by energy dispersive X-ray spectroscopy (EDX). Phase purity is maintained for all the samples as measured by powder X-ray diffraction (XRD). The primary particle size has the most significant effect on the electrochemical performance of the materials with smaller primary particles promoting electrochemical activation and increasing capacity. Discharge capacities exceeding 200 mAh g−1 after 100 cycles at C/3 rate (where 1C = 200 mAh g−1) are consistently obtained over a wide range of operating conditions. Spray pyrolysis is shown to be a promising, robust synthesis technique for the production of Li1.2Mn0.54Ni0.13Co0.13O2 material, delivering excellent electrochemical performance within a wide range of process conditions.