The development of a binder system with a lower carbon footprint as an alternative to Portland cement has been intensely researched. In the present study, alkali-activated fly ash exposed to carbon dioxide at an early age was characterized in compressive strength tests and by MIP, XRD and FT-IR analyses. The compressive strength of carbonated specimens experienced a dramatic increase in comparison to uncarbonated specimens. The microstructural densification of the carbonated specimens was evidenced by MIP. The XRD pattern showed peaks assigned to nahcolite, indicating that the pH was lower in the carbonated specimens. Under the carbon dioxide-rich environment, the aluminosilicate gel reached a more Si-rich state, which improved the mechanical properties of the alkali-activated fly ash.