Barium titanate (BaTiO3) particles were prepared by spray pyrolysis from spray solution containing organic additives. The effects of the type and amount of organic precursors on the crystal structure and morphology of the BaTiO3 particles were investigated. It was found that the morphology of BaTiO3 particles before and after calcination depended on the type of organic additives such as citric acid, ethylene glycol and polyethylene glycol. Among these organic additives, citric acid was the most effective to prepare BaTiO3 particles with nano-structured morphology consisting with uniform size nanometer particles after calcination. It was also found that the phase transformability of the metastable cubic phase to the tetragonal one during calcination could be improved by increasing the content of citric acid in the spray solution. As a result, BaTiO3 particles prepared from spray solution containing high concentration of citric acid had good tetragonality, uniform and fine size, and high BET surface area after calcination. BaTiO3 particles prepared by spray pyrolysis had nanometer size and uniform morphology after simple ball milling process.