Surface images and force measurements obtained using atomic force microscopy (AFM) were used to assess the hydrophobicity of particles from soils and model soil material (smooth glass and acid-washed sand (AWS) exposed to soil-derived humic acid (HA) or lecithin (LE)). Height and phase images, and phase distributions (from soil particles) show complex morphology and heterogeneously distributed organic matter. Forces at model surfaces indicate that, in air, reduction in adhesion corresponded with increased hydrophobicity, but in water, corresponded with a decrease (and serve to guide interpretation of data from natural particles). Adhesion forces on hydrophobic soil particles in water were larger than those for hydrophilic ones, but surface roughness and complexity may obscure any opposite trend for measurements in air. Combination of force measurements, applied forthe first time to soil particles, together with those on model surfaces, and independent assessments of hydrophobicity of corresponding single particle layers, indicate good, but not consistent qualitative agreement between hydophobicity at bulk and nanoscales. AFM is likely to facilitate detailed evaluation of soil particle surface hydrophobicity, which contributes to bulk wetting behavior of soils and other porous systems, including assessments of the potential for contributons to supehydrophobicity from surfaces at the micro- and nanoscales.