A contaminant-free surface of single-crystal alpha-Al2O3 (or sapphire) substrates is key to the experimental studies of its surface and interfacial properties at ambient conditions. Here we critically evaluated methods reported in the literature using comprehensive surface analysis techniques including atomic force microscopy, XPS and contact angle measurements. We found that reported methods did not perform well in terms of removing both organic and particulate contaminants from the (0 0 0 1) basal surface. After thoroughly examining the cleaning effect of various chemical solutions and UV light and plasma irradiation, and based on modified RCA cleaning protocols, we proposed a new wet-cleaning method showing outstanding cleaning performance. This new reliable method will be very useful for the next-step surface chemistry study of single-crystal alpha-Al2O3. It was also demonstrated that AFM, due to its high spatial resolution and sensitivity as a local probe technique, was an indispensable tool for surface contamination control studies. (C) 2013 Elsevier B.V. All rights reserved.