Supersonic spray coating of nanomaterials, owing to high impact velocity of particles, offers significant potential to improve the physical and mechanical properties of target surfaces. Rather than handling individual light nano-scale particles directly with a number of limitations, aqueous nanomaterial colloids and suspensions can be supersonically deposited onto surfaces by converting these complex liquid mixtures into the form of atomized micro-scale droplets. Dispersion and deposition characteristics of these droplets play a vital role in the quality and efficacy of the resultant nanomaterial coating. In the present study, comprising numerical modeling and experimental validation, we investigate details of the dispersion and deposition characteristics of droplets under supersonic flow conditions. In the numerical study, a two-way coupled discrete phase modeling is used to track the discrete phase (i.e., droplets) and to investigate the interaction of droplets with the continuous gas phase (i.e., high-velocity driving gas) in regard to their properties and conditions. The results through computational fluid dynamics (CFD) show that driving gas properties (i.e., temperature, pressure, gas type) and droplet size play a prominent role in droplets dispersion and deposition phenomena. In particular, smaller droplets (≤2 μm) are observed to be more susceptible to turbulent dispersion and evaporation. In the experimental study, an atomization-based supersonic spray system is developed for model validation and a case example of nano-coating applications. The CFD modeling results are validated by particle image velocimetry (PIV) measurements. A case study of titanium dioxide (TiO2) nanomaterial coating on a polymer substrate (ITO/PET film) is performed to demonstrate the suitability of the present spray deposition system, which also addresses the current challenges of TiO2 coating onto ITO/PET surface.