The ability of Pt nanostructures to induce the splitting of the I-I bond in iodine (triiodide) molecules is explored here to enhance electron transfer in the iodine/iodide redox couple. Following the dispersal of Pt nanoparticles at 2% (weight) level, charge transport was accelerated in triiodide/iodide-containing 1,3-dialkylimidazolium room-temperature ionic liquid. If both Pt nanoparticles and multi-walled carbon nanotubes were introduced into the ionic-liquid-based system, a solid-type (nonfluid) electrolyte was obtained. By using solid-state voltammetric (both sandwich-type and microelectrode-based) methodology, the apparent diffusion coefficients for charge transport increased to approximately 1 x 10(-6) cm(2)s(-1) upon the incorporation of the carbon-nanotube-supported iodine-modified Pt nanostructures. A dye-sensitized solar cell comprising TiO2 covered with a heteroleptic Ru-II-type sensitizer (dye) and the semisolid triiodide/iodide ionic liquid electrolyte admixed with carbon-nanotube-supported Pt nanostructures yielded somewhat higher power conversion efficiencies (up to 7.9% under standard reporting conditions) than those of the analogous Pt-free system.