The employment of solid waste, notably coal gangue, in carbon-negative backfill mining technology for mineralization and filling in coal mine gobs, is recognized as a productive method for carbon sequestration and waste management, with research primarily dedicated to engineering advanced mineralized backfill materials. Under this background, four variables, including the ratio of gangue to solids (RG-S), water-cement ratio (RW-C), ratio of fly ash to solid wastes providing calcium (Ca) (RA-Ca), and ratio of flue gas desulfurization (FGD) gypsum to carbide slag (RF-CS) were defined to formulate gangue-based mineralized backfill materials, with orthogonal experiments assessing their effects on CO2 sequestration and mechanical characteristics. The results indicate that RW-C consistently emerges as the primary factor influencing both the amount of sequestered CO2 and the mechanical properties of gangue-based solid waste mineralized backfill materials. The amount of sequestered CO2 demonstrates a direct proportionality to RW-C and mechanical strength demonstrates an inverse relationship with RW-C. After 45 minutes of stirring and carbon sequestration, samples in various groups exhibited an maximum sequestered CO2 amount of 18.96 g·kg−1, with a maximum sequestration rate of 0.20 g·kg−1·min−1. The process of CO2 sequestration enhances the compressive properties of mineralized backfill materials derived from gangue based solid wastes.
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