The present invention provides, in one embodiment, a nanostructured article. In an embodiment, the nanostructured article includes a first material made from a plurality of intermingled nanotubes placed on top of one another to form a continuous structure with sufficient structural integrity to be handled. The nanostructured article can also include a second material made from a plurality of nanotubes forming a layer situated on a surface of the first material. The second material, in an embodiment, has a nanotube density lower than the nanotube density of the first material. The nanostructured article further a layer of ordered pyrolytic carbon between the first material and the second material to enhance the bond and structural integrity between the first material and the second material, as well as enhancing the electrical and thermal conductivity between the first and second materials. A process for forming the nanostructured article is also provided.