The natural bentonite used in this study contained montmorillonite in addition to low cristobalite. The uptake of aqueous Co2+ ions was investigated as a function of time, concentration, and temperature. In addition, the change in the interlayer space of montmorillonite was analyzed using XRPD, and the distribution of fixed Co2+ ions on the heterogeneous clay surface was recorded using EDS mapping. The sorbed amount of Co2+ appeared to closely follow Freundlich isotherm, with the sorption process showing apparent endothermic behavior. The relevance of the apparent _Ho values is briefly discussed. Analysis of the Co-sorbed bentonite samples using SEM/EDS showed that the montmorillonite fraction in the mineral was more effective in Co2+ fixation than the cristobalite fraction. XRPD analysis demonstrated that the interlayer space of montmorillonite was slightly modified at the end of sorption.