A mineral, mimetite Pb5(AsO4)3Cl, is one of the most insoluble minerals and continues to be considered a viable remedial strategy for immobilization of Pb and As from contaminated soils. It has been recognized that many well-known, naturally-occurring, and synthetic chelators strongly influence dissolution processes in near-surface geological environments. In this study, crystals of mimetite were observed in scanning electron microscopy (SEM) and atomic force microscopy (AFM) before and after dissolution in EDTA (ethylene diamine tetra-acetic acid) solution. Direct in situ observations at room temperature made in an AFM fluid cell revealed that the grain surface roughness has increased due to development of etch pits. Both hexagonal and prismatic walls developed dissolution features between 0.6 and 1.2 µm, respectively, during duration of the experiment. AFM observations suggest surface-controlled dissolution dominated step retrieval on both prismatic and hexagonal surfaces. SEM observations showed the development of rounded edges on hexagonal walls and elongated, oval etch pits on the prismatic wall. These results, representing early dissolution patterns on mimetite surfaces, might suggest that low pH conditions in soils containing organic acids similar to EDTA might contribute to remobilization of Pb and As from mimetite when applied to stabilization of these toxic metals in contaminated soils.