Abst ract~he objective of this study was to investigate the influence of layer charge on the hydration of Mg-saturated expandable 2:1 phyllosilicates. Water retained by 12 Mg-saturated clays at 54 % relative humidity was quantified gravimetrically. X-ray diffraction and total chemical analysis were used to de-termine the hydratable surface area (447-759 m z g 1) and layer charge [0.327-0.754 electrons per formula unit (e f.u. ~)] of each sample. Water retained by the clays increased with both hydratable surface area and layer charge of the clays. However, the increase in H20 content with layer charge occurred only on external surfaces of the clays. This result suggests that the H20 on external surfaces is localized around the cation/charge ...