Exfoliated montmorillonite (exMMT) nanoplatelets are a two-dimensional electrolyte carrying ∼1.78 dissociable monovalent cations per nanometer square. They were fabricated through soap-free emulsion polymerization of poly(methyl methacrylate) in the presence of MMT. Because the dissociated exMMTs are anionic, they were not only capable of gelatinizing 1-methyl-3-propylimidazolium iodide (MPII) ionic liquid-based electrolyte, but also increased the power conversion efficiency of resulting dye-sensitized solar cell (DSSC) from 6 to 7.77%. Recently, we investigated the ionic conductive mechanism of exMMT-gelled MPII ionic liquid-based electrolyte and found that the exMMTs acted like an oxidizing agent for iodide ions (I-). As exMMTs were mixed with MPII, I- ions readily oxidized to I3
- and even to I5
- ions by losing the electrons. Consequently, the ionic conductivity was significantly increased due to the fact that I-, I3
-, and I5
- tended to form redox couples that transported faster by way of the Grothus/exchange reaction process.