A B S T R A C T:Two chlorites, sheridanite and clinochlore, have been examined to determine their surface charge characteristics. In order to increase their surface area and to produce a measurable surface charge, the chlorites were treated with 10 -3 M, 10 -2 M, and 10 -l M HCI in 10 -2 M MgC12 solutions. These treatments are shown not to alter the crystallinity of the chlorites and to produce a small pH-dependent negative charge which is not directly related to the total surface area. The clinochlore, (Si6.13A11.84)(A11.53 Femo 9 53 FeIIo. I 8M g9-52) O20(OH) 16, is more readily attacked by the acids than the sheridanite, (Si5.43A12.55)(A12.90FeIIo.05Mg8.86)O20(OH)lr, and also produces material with greater surface area and pH-dependent, negative, surface charge. It is concluded that: (i) isomorphous substitutions in the lattice are not reflected in a permanent surface charge; (ii) the observed surface charge arises not only at the edges of the particles but also at points where the chlorite is predisposed to attack by acids; (iii) in the chlorite-acid system used, anions--probably mainly silicate---block positively charged sites.