In-situ CO2 mineralization of tailings has shown great potential for large-scale CO2 sequestration, but its development is seriously limited by the low CO2 conversion rate. This study proposed an innovative pH swing process to produce activated tailings through magnesium extraction from raw tailings and subsequent leachate precipitation. By the combination of activated tailings and high-belite calcium sulfoaluminate cement, a new type of cemented activated tailings backfill (CATB) was developed. The results demonstrate that 82.33% of magnesium is extracted from raw tailings and precipitates in the form of Mg(OH)2 serving as the dominating carbonation active phase during the pH swing process. Besides the aragonite forms in the carbonated cemented raw tailings backfill (CRTB), carbonated CATB also contains calcite, nesquehonite, and hydromagnesite. Substituting activated tailings for raw tailings led to the higher CO2 absorption capability (ranging from 8.88% to 14.17% with various binder-to-tailings ratios). These indicate that the activated tailings have a promising application scenario in large scale in-situ CO2 mineralization.