Due to their nanometer size and low density, the surface area to mass ratio of carbon nanotubes and carbon nanofibers is extremely large. In addition, the large aspect ratio and high elastic modulus of carbon nanotubes and carbon nanofibers allow for large differences in strain between the constituents in the nanocomposites, which could enhance the interfacial energy dissipation ability. While there are many reported benefits of carbon nanotubes and carbon nanofibers in the nanocomposites, the potential of carbon nanotubes and carbon nanofibers to enhance the structural damping properties of nanocomposites has not been fully explored. This paper presents a novel process to manufacture multifunctional and cost-effective hybrid nanocomposites through integrating engineered carbon nanofiber paper into traditional fiber reinforced composites to improve the structural damping properties. The vacuum-assisted resin transfer molding (VARTM) process was employed to fabricate the nanocomposites by using engineered carbon nanofiber papers as inter-layers or surface layers of traditional composite laminates. To characterize the structural damping properties, the influence of frequency dependence was analyzed through the experiments conducted using the nanocomposite beams. It was found that there is up to 200–700% increase of the damping ratios at higher frequencies. It was found that the connectivities between carbon nanofibers and short glass fibers within the carbon nanofiber paper were responsible for the significant energy dissipation in the nanocomposites during structural vibration applications.

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