We have developed a new method for the fabrication of metal nanoparticle/polythiophene nanotube composites, i.e., the template-based electrochemical polymerization of terthiophene-linked oligoethyleneoxy-thiol (1) and -phosphine (2)-stabilized gold and palladium nanoparticles (1-Au, 1-Pd, and 2-Pd) in a nanoporous alumina membrane as a template gave the nanotube composites (1-Au-PT-NTs, 1-Pd-PT-NTs, and 2-Pd-PT-NTs) of polythiophene and the metal nanoparticles without aggregation of the metal nanoparticles. The nanotube composites were characterized by scanning electron microscopy and transmission electron microscopy. The Pd/polythiophene nanotube composites (2-Pd-PT-NTs) are recyclable highly effective catalysts for carbon-carbon coupling reactions. This new method is currently being extended to other metal and metal oxide nanoparticles/polythiophene nanotube composites to realize a wide range of hybrid nanomaterials with controllable surface chemistry.