Orthoclase (001) surface topography and interface structure were measured during dissolution by using in situ atomic force microscopy (AFM) and synchrotrons X-ray reflectivity at pH 1.1-12.9 and T = 25-84 C. Terrace roughening at low pH and step motion at high pH were the main phenomena observed, and dissolution rates were measured precisely. Contrasting dissolution mechanisms are inferred for low- and high-pH conditions. These observations clarify differences in alkali feldspar dissolution mechanisms as a function of pH, demonstrate a new in situ method for measuring face-specific dissolution rates on single crystals, and improve the fundamental basis for understanding alkali feldspar weathering processes.