During the extraction and utilization of coal resources, a large amount of CO₂ and coal-based solid wastes (CBSW), such as coal gangue, are generated. To reduce the carbon and waste emissions, an effective approach is to mineralize the CO₂ with the CBSW and then backfill the mineralized materials into the goaf area. However, efficient CO₂ mineralization is challenging due to the low reactivity of coal gangue. To this end, mechanical activation was used for the modification of coal gangue, and the mechanical activation mechanism of coal gangue was revealed from a microcosmic perspective by dry powder laser particle size testing (DPLPST), X-ray diffractometer (XRD) analysis, Fourier-transform infrared spectrometer (FTIR) analysis, and scanning electron microscopy (SEM). The results showed that compared with the unground coal gangue, the average particle size of coal gangue after 0.5 h, 1 h, and 1.5 h milling decreases by 94.3%, 95%, and 95.3%, respectively; additionally, the amorphous structures of the coal gangue after milling increase, and their edges and corners gradually diminish. After the pressure mineralization of coal gangues with different activation times, thermogravimetric (TG) analysis was performed, and the CO₂ mineralization effect of the mechanically activated coal gangue was explored. It is found that the carbon fixation capacity of the coal gangue after 0.5 h, 1.0 h, and 1.5 h mechanical activation is increased by 1.18%, 3.20%, and 7.57%, respectively. Through the XRD and SEM, the mechanism of CO₂ mineralization in coal gangue was revealed from a microcosmic perspective as follows: during the mineralization process, alkali metal ions of calcium and magnesium in anorthite and muscovite are leached and participate in the mineralization reaction, resulting in the formation of stable carbonates such as calcium carbonate.