In summary, we adopted a multiscale coarse-grained simulation framework to identify the mechanisms underlying the conductivity characteristics for single-ion conducting nanoparticle-based electrolytes. Our results suggest that for the electrolyte systems studied thus far, the ionic conductivity is dominated by Li + transport along nanoparticle surfaces, in the vicinity of the tethered anions. For such cases, the ionic conductivity is influenced by the connectivity of surface transport pathways and the cation diffusivities in the surface region. The latter in turn depends on the strength of anion-cation interaction and the steric hindrance effects on the mobile charge carrier. We further demonstrate that employing high dielectric constant solvents promotes cation transport through the solvent medium and results in elevated conductivity even at relatively lower nanoparticle loadings.