This study demonstrates, for the first time, the manufacturing of novel nano-nonwovens that are comprised of three-dimensionally distributed carbon nanofibers within the matrices of traditional wet-laid nonwovens. The preparation of these nano-nonwovens involves dispersing and flocking carbon nanofibers, and optimizing colloidal chemistry during wet-lay formation. The distribution of nanofibers within the nano-nonwoven was verified using polydispersed aerosol filtration testing, air permeability, low surface tension liquid capillary porometry, SEM and cyclic voltammetry. All these characterization techniques indicated that nanofiber flocks did not behave as large solid clumps, but retained the 'nanoporous' structure expected from nanofibers. These nano-nonwovens showed significant enhancements in aerosol filtration performance. The reduction-oxidation reactions of the functional groups on nanofibers and the linear variation of electric double-layer capacitance with nanofiber loading were measured using cyclic voltammetry. More than 65 m² (700 ft²) of the composite were made during the demonstration of process scalability using a Fourdrinier-type continuous pilot papermaking machine. The scalability of the process with the control over pore size distribution makes these composites very promising for filtration and other nonwoven applications.