The synthesis, characterization, and catalytic testing of copper and copper:gold nanoparticles in melamine-based dendrons supported on SBA-15 is reported. It was found that by first making small gold nanoparticles using the dendrons as templates, stable copper(0) overlayers could then be successfully deposited. These samples were used as catalysts for the click reaction, with the most active samples possessing rates of 8.9 mol triazole produced/(mol copper - hour), nearly 50 times high than literature reports of copper nanoparticles in solution. In contrast, the gold nanoparticles themselves are inert for this reaction, consistent with the copper being deposited as an overlayer on the gold nanoparticles. Copper leaching was shown to be less pronounced for particles formed in the dendrons versus copper simply deposited on SBA-15. Larger dendrons lead to suppressed rates due to diffusion resistance with rates decreasing from 8.9 to 5.2 to 0.69 mol triazole produced/(mole Cu-hour) for G1, G2, and G3 respectively. Infrared spectroscopy was used to monitor the reaction in real time, and provided information about the various surface intermediates formed.