Clay minerals are likely candidates to aid in nuclear waste isolation due to their low permeability, favorable swelling properties, and high cation sorption capacities. Iodine-129 is often the major driver of exposure risk from nuclear waste repositories at timescales > 10, 000 years. Therefore, understanding the geochemical cycling of iodine in clays is critical in developing defensible quantitative descriptions of nuclear waste disposal. Seven different clay minerals have been examined using several techniques to characterize the surface charge environment and iodide uptake. The use of a series of clays shifts the independent variable away from water chemistry characteristics (pH, contaminant concentration), and toward structural characteristics of clay minerals including isomorphous substitution and clay texture. Iodide uptake batch experiments were completed with the clay minerals in a range of swamping electrolytes. The results give evidence for a novel uptake mechanism involving ion pair formation and iodide concentration within nano-confined environments.