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This paper presents a fundamental study of processing, morphologies, properties, and applications of a novel non-woven nanopaper based on carbon nanofibers (CNFs). Unique material formulations were developed to tailor the non-woven nanopaper to specific engineering applications. The non-woven nanopaper was made from a variety of nanomaterials (e.g. carbon nanotubes, carbon nanofibers, graphene, nanoclay, nickel nanostrands, POSS, etc.) with tailored nanostructures by precisely controlling composition, dispersion, functionalization, orientation, porosity, and thickness during the vacuum infiltration, pressure infiltration, or spray/infiltration process. The polymer matrix was impregnated into the stacked nanopapers to form multi-layered laminated composites. Such non-woven nanopaper based composites were designed and fabricated to achieve high energy dissipation capability for vibrational damping, high thermal conductivity and thermal stability for fire retardancy, ultra-high electrical conductivity and current-carrying capacity for lightning strike protection, and electro-actuation of shape memory polymer composites.