Carbon nanotubes are one of the most prominent materials in research for creating electrodes for portable electronics. When coupled with metallic nanoparticles the performance of carbon nanotube electrodes can be dramatically improved. Microwave reduction is an extremely rapid method for producing carbon nanotube-metallic nanoparticle composites, however, this technique has so far been limited to carbon nanotube soot. An understanding of the microwave process and the interactions of metallic nanoparticles with carbon nanotubes have allowed us to extend this promising functionalisation route to pre-formed CNT electrode architectures. Nanoparticle reduction onto preformed architectures reduces metallic nanoparticle waste as particles are not formed where there is insufficient porosity for electrochemical processes. A two-fold increase in capacitive response, stable over 500 cycles, was observed for these composites, with a maximum capacitance of 300 F g À1 observed for a carbon Nanoweb electrode.Next-generation nanostructured electrochemical devices are anticipated to play a key role in future portable electronics. Components of these devices such as supercapacitors and lithium-ion batteries have attracted intense research effort. Carbon is a widely studied electrode material due to its broad abundance, ease of processing, and variety of allotropes. Of these allotropes, carbon nanotubes (CNTs) have proved theoretically to be one of the most promising electrode materials to date. 1,2 CNTs demonstrate phenomenal physical properties, 3,4 which make them excellent materials for use as high performance electrodes in a variety of applications. 5,6 CNT/amorphous carbon mats or 'buckypapers' are one such example of a CNT electrode structure. 7,8 Recently, the authors have reported on the