The mechanochemical activation of a high defect kaolinite has been studied using a combination of high-resolution thermogravimetry and DRIFT spectroscopy. The effect of grinding causes a decrease in the dehydroxylation temperature and an increase in the amount of adsorbed/coordinated water. The temperature of dehydration also increases with grinding time. It is proposed that this dehydroxylation occurs through a homogenous process involving proton transfer through point heating. The amount of adsorbed water decreases with the increase in temperature of the thermal treatment