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This study aims to formulate solid and aqueous compositions of hydrated Portland cement incorporated with reactive alumina (RA) via thermodynamic modeling, with the goal to prevent alkali–silica reaction (ASR). Based on SEM/EDS point analysis, the uptake of Al into C–S–H was corrected in the thermodynamic modeling to improve the accuracy. The predicted solid and aqueous compositions were validated by means of XRD, TGA, and ICP. An accelerated mortar bar test was also carried out to confirm the ASR mitigating efficiency, and a preliminary relationship among the ASR expansion, solid assemblage, and aqueous species was established. The critical content for RA is around 5.75% in the studied systems, above which katoite precipitates, resulting in increased Al concentration in the pore solution (∼0.8 mmol/L); hence, ASR can be effectively inhibited. [ABSTRACT FROM AUTHOR]