The present invention provides electrodes comprised of metal-coated vertically aligned carbon nanofibers. Arrays of vertically aligned carbon nanofibers provide highly accessible, high density templates having large electrochemically active surface areas that may be modified to further increase the surface area of the nanofibers. The methods of the present invention involve functionalizing the surface of the nanofibers and coating the functionalized surface with metal using electroless deposition. The resulting metal-coated nanofibers form highly stable and highly reproducible electrodes having very high surface areas. The electrodes of the present invention are expected to be useful in a variety of applications, including high-density energy storage, i.e., supercapacitors and fuel cells.
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