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Mineral carbonation is emerging as a reliable CO2 capture technology that can mitigate climate change. In lime-treated clayey soils, mineral carbonation occurs through the carbonation of free lime and cementitious products derived from pozzolanic reactions. The kinetics of the reactions in lime-treated clayey soils are variable and depend primarily on soil mineralogy. The present study demonstrates the role of soil mineralogy in CO2 capture and the subsequent changes caused by carbon mineralization in terms of the unconfined compressive strength (UCS) of lime-treated soils during their service life. Three clayey soils (kaolin, bentonite, and silty clay) with different mineralogical characteristics were treated with 4% lime content, and the samples were cured in a controlled environment for 7 d, 90 d, 180 d, and 365 d. After the specified curing periods, the samples were exposed to CO2 in a carbonation cell for 7 d. The non-carbonated samples purged with N2 gas were used as a benchmark to compare the mechanical, chemical-mineralogical, and microstructure changes caused by carbonation reactions. Experimental investigations indicated that exposure to CO2 resulted in an average increase of 10% in the UCS of lime-treated bentonite, whereas the strength of lime-treated kaolin and silty clay was reduced by an average of 35%. The chemical and microstructural analyses revealed that the precipitated carbonates effectively filled the macropores of the treated bentonite, compared to the inadequate cementation caused by pozzolanic reactions, resulting in strength enhancement. In contrast, strength loss in lime-treated kaolin and silty clay was attributed to the carbonation of cementitious phases and partly to the tensile stress induced by carbonate precipitation. In terms of carbon mineralization prospects, lime-treated kaolin exhibited maximum carbonation due to the higher availability of unreacted lime. The results suggest that, in addition to the increase in compressive strength, adequate calcium-bearing phases and macropores determine the efficiency of carbon mineralization in lime-treated clayey soils.