This paper describes a collaborative theoretical and experimental research effort to investigate both the atomization dynamics of non-Newtonian liquids as well as the performance of coaxial atomizers utilized in pharmaceutical tablet coating. In pharmaceutically relevant applications, the coating solutions being atomized are typically complex, non-Newtonian fluids which may contain polymers, surfactants and large concentrations of insoluble solids in suspension. The goal of this investigation was to improve the understanding of the physical mechanism that leads to atomization of viscous and non-Newtonian fluids and to produce a validated theoretical model capable of making quantitative predictions of atomizer performance in pharmaceutical tablet coaters. The Rayleigh–Taylor model developed by Varga et al. has been extended to viscous and non-Newtonian fluids starting with the general dispersion relation obtained by Joseph et al. The theoretical model is validated using droplet diameter data collected with a Phase Doppler Particle Analyzer for six fluids of increasing rheological complexity. The primary output from the model is the Sauter Mean Diameter of the atomized droplet distribution, which is shown to compare favorably with experimental data. Critical model parameters and plans for additional research are also identified.