Spherical Ni0.5Mn0.5CO3 is synthesized via carbonate co-precipitation method which uses NH4HCO3 as the precipitator. However, obvious agglomerate of secondary particles occurs when NH4HCO3 is used as the precipitator. The agglomerate particles can result in inferior physical characteristic. An improved carbonate co-precipitation which used NH4HCO3 doped with different proportion of NaOH as a new precipitator is tested in our study. Observed by SEM and Mastersizer, spherical morphology with narrow particle size distribution is synthesized with the proportion of NaOH reaches 10%. The element line analysis by Electron Probe Micro-analyzer shows symmetrical distributions of Ni and Mn elements via the improved carbonate co-precipitation.