Alkali-activated cements prepared from aluminosilicate powders, such as blast furnace slag and fly ash, are rapidly attracting attention as alternatives to cement because they can significantly reduce CO₂ emissions compared to conventional cement concrete. In this study, we investigated the relationship between the physical and chemical changes by accelerated carbonation conditions of alkali-activated cements. Alkali-activated cements were prepared from binders composed of blast furnace slag and fly ash as well as alkali activators sodium silicate and sodium hydroxide. Physical changes were analyzed from compressive strength, pH, and neutralization depth, and chemical changes were analyzed from XRD, TG-DTG, and ²⁹Si MAS NMR. The C–(N)–A–S–H structure is noted to change via carbonation, and the compressive strength is observed to decrease. However, in the case of Na-rich specimens, the compressive strength does not decrease by accelerated carbonation. This work is expected to contribute to the field of alkali-activated cements in the future.