The role of magnesium oxide (MgO) in the carbonation of cementitious materials, particularly alkali-activated materials (AAM), which is a promising low-carbon alternative to ordinary Portland cement (OPC), has garnered significant attention. However, there remains a lack of clear understanding regarding its underlying mechanisms and interrelation with calcium oxide (CaO) content. This study aims to understand the influence of MgO on carbonation mechanisms, carbonation products, and (C, N)–A–S–H gel micromechanical properties in AAM. Four different binder formulations were examined by varying contents of slag, class F fly ash, and light-burned MgO. A powder-type sodium metasilicate was used as an alkaline activator. CO2 curing was conducted in a CO2 incubator with 1 % concentration and under atmospheric pressure for up to 56 days using pulverized paste binders. The carbonation mechanism, polymorphs of carbonation products, and the micromechanical properties of the (C, N)–A–S–H gel matrix were characterized by conducting laboratory tests including pH measurement, XRD, TGA, DSC, nitrogen adsorption, and nanoindentation at various carbonation stages. A noticeable pattern of pH initially dropping and then rising was observed. Integrated XRD-TGA demonstrated the evolution, polymorphism, and amount of calcium carbonate phases. Higher MgO content in AAM binders favored the formation of aragonite and hydrotalcite. Extensive nanoindentation results and their statistical analysis revealed binder-specific trends in the pozzolanic matrix stiffness before and after carbonation. The findings of this study can be used in developing AAM binders as building materials and to provide a deeper understating of the carbonation reactions in AAM binders.