The physical property requirements for kaolinite suspensions to display time-dependent structural rebuilding or rejuvenation behavior are the same as required by smectite gels such as hectorite and Na-montmorillonite (NaMnt), a rare discovery linking the two types of clay. A holistic framework for predicting clay gel behavior based on the clay physical properties such as charge, crystal structure, and mineralogy, may emerge and was the ultimate goal of this research. A structural rejuvenation process during both ageing and stepdown shear rate modes was postulated to require that the silica and alumina faces of the kaolinite platelets be negatively charged to produce a strong electric double layer (EDL) repulsion in all face-face configurations. This is needed to slow down the (+)edge to (–)face bonding process to produce the time-dependent behavior. Currently, the unlike charge attraction between the silica and alumina faces makes the structural rebuilding process of a pre-sheared kaolinite suspension too fast to be observable. Two methods of making the alumina face negatively charged, i.e. the use of adsorbed P2O74– and high pH, did indeed produce the time-dependent behavior for both KGa-1b and KGa-2 suspensions, thus validating the proposed hypothesis. The KGa-1b with a lower content of octahedral positive layer charge required less P2O74– and a lower pH to achieve the desired outcome. Addition of 0.002 M NaCl to the high pH-treated KGa-2 suspension hastened the structural rejuvenation process and increased the aged gel strength. The oscillatory behavior in the stepdown shear stress at low pH was due to layer agglomerates formed by (+)face to (–)face attraction. Bulky layered agglomerates were reduced markedly by both the P2O74– and high pH treatments. The knowledge gained was applied successfully to make clay-rich iron ore tailings time-dependent in both the ageing and stepdown shear rate modes.