A mathematical model was developed for spray pyrolysis to produce hollow spherical ceramic particles. The mechanism was established based on the previous experimental results. The transfer of mass, momentum, and heat inside and around the aerosol droplets was considered simultaneously. Simulation was carried out to study the effects of operating parameters on the quality of derived particles. The simulated and experimental results were in agreement and showed that: (a) raising the pyrolysis temperature increased the size and size distribution of resultant particles, and decreased the specific surface area and the bulk density; (b) lowering the concentration of starting solution decreased the size and size distribution of resultant particles, and increased the specific surface area and bulk density.