Aerosol coating processes were developed to deposit titania ceramic films onto steel and silica substrates. In situ lightscattering measurements were used to understand the deposition mechanisms in different system configurations. The conditions that were necessary to obtain uniform, nonporous, and well-adhered titania films on steel substrates were established. The as-coated films had excellent anticorrosion characteristics at room temperature, as established by the standard salt-fog test. Film crystallinity and morphology were examined using X-ray diffractometry and scanning electron microscopy; these analysis methods revealed an oriented, nanocrystalline anatase phase. Film composition was established, as a function of film thickness, using Auger electron spectroscopy and was confirmed to be stoichiometric (Ti:O = 1:2). The optical band gap and optical phonons of the deposited films were probed using spectrophotometry and Raman scattering, respectively; these analysis methods revealed a blue shift of the gap, relative to bulk anatase, and a localization of carriers in the nanometer-sized crystallites.