Chlorite is a layered silicate mineral group of importance in geology, agriculture, and in the processing of mineral resources. A more detailed analysis of the surface charge of chlorite minerals is important in order to improve our fundamental understanding of such particle structures and their behavior in suspension. In this study, the anisotropic surface charging of chlorite has been established using Atomic Force Microscopy surface-force measurements with a silicon nitride tip. The surface-charge densities and surface potentials at the chlorite basal-plane surfaces and edge surface were obtained by fitting force curves with the Derjaguin-Landau-Verwey-Overbeek theoretical model. The results show that at pH 5.6, 8.0, and 9.0 the chlorite mica-like face is negatively charged with the isoelectric point (IEP) less than pH 5.6. In contrast, the chlorite brucite-like face is positively charged in this pH range and the IEP is greater than pH 9.0. The surface charging of the chlorite edge surface was found to be pH-dependent with the IEP occurring at pH 8.5, which is slightly greater than the edge surfaces of talc and muscovite due to the larger content of magnesium hydroxide at the chlorite edge surface. Findings from the present research are expected to provide a fundamental foundation for the analysis of industrial requirements, e.g. collector adsorption, slime coating, and particle interactions in the area of mineral-processing technology.