Novel freestanding foils of vertically aligned carbon nanotube arrays (VANTAs) fused with metals are fabricated in a scalable four-step process of (1) VANTA synthesis, (2) deposition of partially infused metal film, (3) removal from growth substrate, and (4) optional deposition of a second metal film on the back side. Mechanical and electrical testing demonstrates excellent contact between the VANTA and the interface-infused metal layers.