We report on morphosynthesis techniques that have been employed to tune polyamine film nanoarchitectures and on their resulting morphologies. Specific layers discussed include films of aniline/Laponite clay and aniline solution processed with V 2 O 5 catalyst. Synthesis approaches examined include films generated in-situ (glass templating), solution based drop casting, and mechanochemical grinding. Surface topography results suggest that these approaches provide dimensionality control of the polyaniline morphology. Surface images of the mechanochemically ground polyaniline/Laponite nanocomposite layer reveal interfacial contact which is promising for potential heterojunction solar cell designs.