The oil-sand ores of northern Alberta provide a significant proportion of the overall energy portfolio for North America. Surprisingly, the presence of nano-sized clay minerals plays a defining role both in the extraction of bitumen and in tailings management. Although seemingly insignificant in size, naturally occurring clay minerals present in the oil sand ores of northern Alberta create significant challenges in all aspects of bitumen extraction and recovery, processing of oil sand ores, and management of tailings. Although a significant body of knowledge exists in relation to the characterization of ‘oil-sands clay minerals,’ much of this work has focused on the identification of the clay minerals present and not on their respective surface chemistries. This chapter focuses on some of the unique structural features of the clay minerals found in the oil sands and their respective surface chemistries.