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Spontaneous combustion coal gangue (SCCG) is considered to be an aluminosilicate-based solid waste containing various toxic ions. The alkali-activation method for this material can not only fully use its potential hydration activity but also solidify the hazardous components to some extent. Through introducing additional Pb2+, the solidification behavior of heavy metal Pb2+ for an SCCG-based geopolymer was studied in the present paper. The solidification efficiencies were evaluated by Pb2+ leaching rates under neutral and acidic conditions, while its mechanism was explained by the methods of XRD, TG, FT-IR, SEM, and MIP. The results show that the Pb2+ solidification efficiency increases along with the curing age, and acidic rather than neutral conditions lead to a more intensive solidification capacity. Judging by the permissive maximum value of 5 mg/L, the Pb2+ original concentrations under neutral and acidic circumstances should be lower at 2.0 wt.% and 3.0 wt.%, respectively. The Pb2+ absorption is dominated by the physical process, due to the formation of no new hydration products. However, the Pb2+ addition would interrupt the reconstruction of the Si-Al network structure, slowing the accumulation of N-A-S-H gel and the densifying of the matrix. When the Pb2+ concentration grows, the sizes of hydration productions shrink continuously, more defects appear in the microstructure of the geopolymer, and the pore structure deteriorates rapidly, all of which accelerate the diffusion of toxic ions to the external condition. [ABSTRACT FROM AUTHOR]