Alkali-silica reaction (ASR) has emerged as one of the major concrete deterioration issues. Despite the extensive effort investments in ASR mitigation, the interaction between ASR and carbonation remains unclear. To investigate the role and mechanisms of early-age enforced carbonation in ASR, enforced carbonation conditions at 50 °C and 95 % RH with different CO2 concentrations up to 20 % were employed at two stages. The ASR mitigation efficacy was evaluated by monitoring the volume expansion and cracking behavior of mortars containing reactive aggregates. A comprehensive understanding was obtained by analyzing the evolutions of ASR gel's composition, molecular structure, and hygroscopicity. The results indicate that ASR can be effectively suppressed under carbonation with a 97.9 % decrease in ASR-induced volume expansion and fully suppressed cracking when the mortars were cured at 20 % CO2 for 30 days. The decreases in the Q3 polymerization sites and [K + Na]/Si ratios of the ASR products, as well as the 30.3 % reduction in water uptake capacity of ASR gels under carbonation, uncovered the underlying mechanisms for the mitigated ASR at multiple length scales.