Exploiting the superior properties
of nanomaterials at macroscopic scale is a key issue of nanoscience.
Different from the integration strategy, “additive synthesis”
of macroscopic structures from nanomaterial templates may be a promising
choice. In this paper, we report the epitaxial growth of aligned,
continuous, and catalyst-free carbon nanofiber thin films from carbon
nanotube films. The fabrication process includes thickening of continuous
carbon nanotube films by gas-phase pyrolytic carbon deposition and
further graphitization of the carbon layer by high-temperature treatment.
As-fabricated nanofibers in the film have an “annual ring”
cross-section, with a carbon nanotube core and a graphitic periphery,
indicating the templated growth mechanism. The absence of a distinct
interface between the carbon nanotube template and the graphitic periphery
further implies the epitaxial growth mechanism of the fiber. The mechanically
robust thin film with tunable fiber diameters from tens of nanometers
to several micrometers possesses low density, high electrical conductivity,
and high thermal conductivity. Further extension of this fabrication
method to enhance carbon nanotube yarns is also demonstrated, resulting
in yarns with ∼4-fold increased tensile strength and ∼10-fold
increased Young’s modulus. The aligned and continuous features
of the films together with their outstanding physical and chemical
properties would certainly promote the large-scale applications of
carbon nanofibers.