A thermal interface material includes a mechanically compliant vertically aligned nanofiber film and a binder material for joining the nanofibers of the film to the surfaces of two substrates. Preferably, the binder material comprises a non-hydrocarbon-based material such as a metallic eutectic with a melting temperature below a nanofiber thermal damage threshold temperature of the film. The film is grown on a substrate which is then bonded to another substrate by the binder material in an adhesion process that may include pressure and heat. Alternatively, the film may be released from the substrate to produce a stand-alone thermal tape which may later be placed between two substrates and bonded.