Enhanced mass transfer rates have been frequently observed in diffusion studies with alkaline and earth alkaline elements in compacted clay minerals and clay rocks. Whether this phenomenon, often termed surface diffusion, is also relevant for more strongly sorbing species is an open question. We therefore investigated the diffusion of Sr2+, Co2+ and Zn2+ in compacted illite with respect to variations of the concentration of the background electrolyte, pH and carbonate. A dependence of the effective diffusion coefficients on the concentration of the background electrolyte was observed for all three elements. A similar correlation was found for the sorption distribution ratio (Rd) derived from tracer breakthrough in the case of Sr2+, while this dependence was much weaker for Co2+ and Zn2+. Model calculations using Phreeqc resulted in a good agreement with the experimental data when it was assumed that the cationic species, present in the electrical double layer (EDL) of the charged clay surface, are mobile. Species bound to the specific surface complexation sites at the clay edges were assumed to be immobile. The normal approach of deriving unknown effective diffusion coefficients from reference values of an uncharged water tracer may significantly underestimate the mobility of metal cations in argillaceous media.