A simple route to assemble liquid exfoliated few-layer graphene (GR) and single wall carbon nanotubes (SWCNTs) at the interface between two immiscible electrolytic solutions (ITIES) is reported. The electrochemical reactivity of these interface-assembled low dimensional carbon films was probed by model redox species. The ITIES is also shown to be an ideal substrate for the generation of metal nanoparticles on such conducting nano-carbon supports: this approach is exemplified using the electro-deposition of palladium nanoparticles on the free-standing GR and SWCNT layers.