Several proposed mechanisms of the thixotropic behavior of montmorillonite‐water systems were evaluated. The effects of temperature, reshearing, concentration, and storage time on these systems were studied by means of NMR and rheological measurements. The specific parameters used were the change in line width of the NMR spectrum and the static yield values obtained from the rheograms. The results indicate clear agreement with the theory that the colloidal particles upon contact adhere to form a spacious matrix resembling a house of cards. Copyright © 1969 Wiley‐Liss, Inc., A Wiley Company