Coal gangue is one of the industrial solid wastes that may harm the human body through the ecosystem for a long time. Using coal gangue in geopolymer preparation can effectively reduce cement output and meet the sustainability requirements. In this paper, the physical and chemical characteristics, including the heavy metal content, of coal gangue from different producing areas are described. Then, the mechanism of physical activation (mechanical and thermal activation), chemical activation, and compound activation of coal gangue are illustrated. The machinability, as well as the mechanical, microscopic, and toxicity consolidation properties of geopolymers prepared from coal gangue, are summarized and analyzed. The results indicate that the coal gangue geopolymers can have higher mobility and mechanical strength than cement-based composites by adjusting high calcium element material, alkali activator content, Na2SiO3 modulus, and curing condition. After physical activation, coal gangue is used in geopolymer preparation with a chemical activator (alkali excitation agent), which effectively forms a three-dimensional silicon aluminate polymer network. The pore structure is dense, the physical fixation and chemical bonding are strengthened, and the solidification and adsorption of heavy metal ions are improved. Further, it can also be applied to solidifying radioactive waste, which is following the future development direction.