Fourteen Canadian clays and clay admixtures were subjected to simulated nuclear waste repository environments. The present work is concerned with the montmorillonite-dominant materials only. The montmorillonite-dominant samples showed significant leaching on interaction with deionized water. On heating the samples at 200°C for 500 hours, montmorillomites lost intermicellar water completely and acquired cusp-like to cylindrical morphologies. The loss of water and the morphological changes in montmorillonites significantly altered the engineering characteristics. Permeability, shrinkage limits, compactability and shear strength varied in response to the dominant exchange cation in the structure of montmorillonites and the presence of other mineral components in the materials. The synthetic granite water reacted with montmorillonites and led to changes in chemical and mineralogical compositions, crystalline state and engineering properties.