Atomic force microscopy (AFM) is capable of solid surface characterization at the microscopic and submicroscopic scales. It can also be used for the determination of surface tension of solids (gamma) from pull-off force (F) measurements, followed by analysis of the measured F values using contact mechanics theoretical models. Although a majority of the literature gamma results was obtained using either Johnson-Kendall-Roberts (JKR) or Detjaguin-Muller-Toporov (DMT) models, re-analysis of the published experimental data presented in this paper indicates that these models are regularly Misused. Additional complication in determination of gamma values using the AFM technique is that the measured pull-off forces have poor reproducibility. Reproducible and meaningful F values can be obtained with strict control over AFM experimental conditions during the pull-off force measurements (low humidity level. controlled and known loads) for high quality substrates and probes (Surfaces Should be free of heterogeneity, roughness, and contamination). Any probe or substrate imperfections complicate the interpretation of experimental results and often reduce the quality Of the generated data. In this review, surface imperfection in terms of roughness and heterogeneity that influence the pull-off force are analyzed based upon the contact mechanics models. Simple correlations are proposed that Could guide in selection and preparation of AFM probes and Substrates for gamma determination and selection of loading conditions during the pull-off force measurements. Finally, the possibility of AFM measurements of solid Surface tension using materials with rough Surfaces is discussed. (C) 2004 Elsevier Inc. All rights reserved.