While the mechanisms underlying ion transport in lithium-salt doped nanocomposite electrolytes have been examined, those governing ion transport in the newer class of nanoparticle-based single-ion conducting electrolytes remain poorly understood. Notably, the origins of an optimal nanoparticle loading for (maximizing) ionic conductivity and the pronounced influence that modifying the nanoparticle-tethered counterions has on the magni-tude of the conductivity 15 are still unresolved. Further, these properties motivate questions regarding the potential of such materials to conduct alternative cations and the possible avenues for enhancing their ionic conductivity.