With the growing demand for unique multifunctional composite materials for a range of advanced applications, there is a need for scalable fabrication processes that would allow for precise nanostructure control. The soft lithography technique, Particle Replication in Non-wetting Templates (PRINT), is a viable approach for this type of fabrication. PRINT utilizes perfluoropolyether (PFPE) elastomeric molds to generate ordered arrays of monodisperse, shape-specific particles. Thus, it provides complete tunability of the filler particle parameters: shape, size (nanometer to micron), orientation and composition. With this approach, particles are arranged in a polymer matrix to generate complex three dimensional architectures, where particles cannot aggregate. Both polymer-polymer and polymer-ceramic composites have been generated using this technique, with particle inclusions ranging in size from 7 micron to 200 nm. The polymer-polymer composites have been prepared with thermoplastic particle inclusions, such as polyvinylpyrrolidone, polystyrene, and the semi-conducting polymer, poly[2-methoxy-5-(3,7-dimethyloctyloxy)-1,4-phenylenevinylene] (MDMO-PPV). Crosslinked particles, such as poly(trimethylolpropane ethoxylate triacrylate), were also incorporated into the composites. Most of the samples were prepared with crosslinked matrices, such as poly(ethylene glycol) (PEG), epoxy, and PFPE. Two examples of polymer-ceramic composites that have been fabricated with controlled microstructure are PFPE-barium titanate (PFPE-BaTiO3) and PFPE-cadmium oxide (PFPE-CdO). SEM and optical microscopy are used to image the composite films. Efforts are currently focused on the optimization of the fabrication process, and the characterization of the electrical and optical properties of the multilayered composite films.