The alkalinity of CaO is commonly insufficient in alkali-activating raw soils or minerals for the formation of cementation or geopolymerization. In this study, nonthermal plasma (NTP) irradiation was employed to activate traditional CaO to enhance its efficacy in alkali activation and further intensify the self-cementation of gold tailings. The solidification/stabilization (S/S) of the gold tailings-based matrix activated by NTP-CaO was better than that of CaO. The NTP irradiation enhanced the surface hydroxyl groups and oxygen atoms, decreased...