HYPOTHESIS: Multicomponent coatings with layers comprising different functionalities are of interest for a variety of applications, including electronic devices, energy storage, and biomaterials. Rather than creating such a film using multiple deposition steps, we explore a single-step method to create such films by varying the particle Peclet numbers, Pe. Our hypothesis, based on recent theoretical descriptions of the stratification process, is that by varying particle size and evaporation rate such that Pe of large and small particles are above and below unity, we can create stratified films of polymeric and inorganic particles. EXPERIMENTS: We present AFM on the surface composition of films comprising poly(styrene) nanoparticles (diameter 25-90 nm) and silica nanoparticles (diameter 8-14 nm). Previous studies on films containing both inorganic and polymeric particles correspond to large Pe values (e.g., 120-460), while we utilize Pe ∼ 0.3-4, enabling us to test theories that have been developed for different regimes of Pe. FINDINGS: We demonstrate evidence of stratification and effect of the Pe ratio, although our results agree only qualitatively with theory. Our results also provide validation of recent theoretical descriptions of the film drying process that predict different regimes for large-on-top and small-on-top stratification.