High-sulfur mixed fly ash residues from semi-dry flue gas desulfurization units in coal-fired power plants are unsuitable for use as supplementary cementitious material (SCM) for concrete production or carbon dioxide utilization. In this work, we explore the potential for upcycling a representative spray dry absorber ash (10.44 wt% SO<
sub>
3<
/sub>
) into concrete-SCM by selective sulfur removal via weak acid dissolution while simultaneously exploring the possibility for CO<
sub>
2<
/sub>
capture. Towards this effort, parametric studies varying liquid-to-solid ratio, acidity, and CO<
sub>
2<
/sub>
pressure were conducted in a batch reactor to establish the sulfur removal characteristics in de-ionized water, nitric acid, and carbonic acid, respectively. The dissolution studies show that the leaching of sulfur from calcium sulfite hemihydrate, which is the predominant S phase, is rapid and achieves a concentration plateau within 5 min, and subsequently, appears to be controlled by the primary mineral solubility. Here, preferential S removal was sufficient to meet SCM standards (e.g., 5.0 wt% as per ASTM C618) using all three washing solutions with 0.62?0.72 selectivity (S^), defined as the molar ratio of S to Ca in the leachate, for a raw fly ash with bulk S^ = 0.3. Acid dissolution with 1.43 meq/g of ash or under 5 atm CO<
sub>
2<
/sub>
retained >
18 wt% CaO and other Si-, Al-rich phases in the fly ash. Based on the experimental findings, two sulfur removal schemes were suggested for either integration with CO<
sub>
2<
/sub>
capture and utilization processes using flue gas or to produce fly ash for use as a SCM.