Controlled, plasma-mediated, surface modification of various substrates including inorganic and organic polymers is essential for the creation of miniaturized advanced materials. Many of these approaches have focused on the surface-implantation of specific chemical groups which can be employed for subsequent chemical reactions where molecular recognition plays a significant role (e, g, immobilization of biomolecules; preparation of catalysts, etc.). The deposition of predesigned-structure thin macromolecular layers on various substrate surfaces is another branch of surface modification processes. By creating high specificity surface layers (e. g. chemically inert films, electrically insulating layers, etc.) on commodity materials will open up routes for the development of economical future technologies. In this contribution some of the recent results, generated at the Center for Plasma-Aided Manufacturing, University of Wisconsin-Madison, in the field of RF-plasma-mediated surface deposition and functionalization processes are discussed.