113Cd solid-state nuclear magnetic resonance (NMR) was used to identify possible Cd2+ adsorption sites in montmorillonite. The montmorillonite was treated with 0.1 and 1 M CdCl2 aqueous solutions and samples with 13 and 8-µm particle size were used. The data are consistent with a two-site model for sorption of Cd2+ on montmorillonite. Cd2+ is localized in the montmorillonite in two different sites: 1) in the interlayers as hydrated Cd2+ and 2) on the external surface, probably with few H2O molecules hydrating to it. Cadmium is also adsorbed as CdCl+ in the interlayer. Treatment with a 0.1 M CdCl2 solution produces adsorption of free Cd2+ in the interlayer whereas treatment with 1 M CdCl2 resulted in adsorption of Cd2+ in both the interlayer and on surface sites and the adsorption of CdCl+ in the interlayer. A larger particle size favors Cd2+ adsorption on the external surface whereas a smaller particle size favors Cd2+ adsorption in the interlayer.