Four types of BaTiO3 powders are prepared and successfully deposited on glass and Pt/Si substrates using the aerosol deposition process. Particles with sizes of 0.45 μm and 0.3 μm are selected as the starting powder, while those powders are treated using a different milling method. The jet-milled and ball-milled powders not only showed a smaller particle-size distribution, but compared with the non-milled powder, it also had a higher deposition rate using the uniformly generated aerosol. Although the films deposited using particles with size 0.45 μm exhibited some craters on the surface, significantly flat film surfaces were obtained. However, particles with size 0.3 μm create a slightly rough film surface, but the dielectric constant was greater than in the case involving particles with size 0.45 μm. Consequently, a suitably large particle size significantly influences the deposition rate and improvement in the surface roughness, and a uniform particle size distribution appears to contribute to an improved dielectric constant. Therefore, it is believed that the dielectric properties along with the growth characteristics can be enhanced by limiting particle size and shape.