We fabricated a highly conductive pyrolytic carbon layer that penetrates into nanoporous alumina channels and that strongly adheres to an aluminum (Al) current collector in order to reduce the contact resistance at the interface between a carbon active material and an Al current collector. The fabrication method includes the following processes: (i) Al anodization, (ii) alumina etching, (iii) nickel seed layer deposition on the alumina surface, and (iv) chemical vapor deposition of pyrolytic carbon grown by the catalytic nickel layer. From SEM and EDX analyses, we confirmed that the pyrolytic carbon could be uniformly placed into an alumina nanoporous template on the Al substrate. Based on measurements of the transverse resistance and electrochemical capacitor tests, the fabricated composite layer of pyrolytic carbon and nanoporous alumina significantly reduced contact resistance of Al/carbon interface due to the highly conductive pyrolytic carbon formed through the nanoporous alumina on the Al surface.