Abstract: The partial molar free energies, entropies and heat contents of the water in suspensions of Li-, Na-, and K-clay were measured relative to pure water by means of a tensiometer. This method of obtaining these thermodynamic properties is far more sensitive than the more common method utilizing adsorption isotherms and a form of the Clausius-Clapeyron equation. The partial molar free energy of the water decreased with time after stirring and increased rapidly upon stirring. This was taken as evidence that a gradual increase in the degree of orientation of water molecules associated with the clay particles occurred as the particles fell into the more random edge-to-surface thixotropic structure. The partial molar entropies and heat contents of the water in the suspensions were found to be less than those for pure water. Hence, this evidence also supported the postulate that an ordered water structure exists in the thixotropic suspensions.