Mineralization of gaseous carbon dioxide into solid carbonates using alkaline industrial residues such as coal fly ash has a dual advantage of reducing the carbon dioxide footprint of coal power plants and improving ash utilization. However, the slow mineral carbonation rate under atmospheric conditions is a major challenge, especially when using natural minerals or industrial residues for direct air capture (DAC) of CO2. In this study, using coal fly ash samples and concentrated alkali carbonate aqueous solutions as a recyclable solvent, we show the feasibility of coupling mineral carbonation with DAC under atmospheric conditions. Findings show that carbonation efficiency is best under alkaline conditions, achieving as high as ∼80% conversion to calcium carbonates within 1 h in a 1.9 M sodium carbonate solution. Based on the experimental results, a process coupling DAC and mineral carbonation that operates entirely under ambient conditions is proposed. The techno-economic and life cycle assessments for the proposed process project a levelized cost of $116–133/t-CO2-sequestered (US $2019) and process carbon emissions (GWP) in the range of 0.03–0.25 t-CO2e/t-CO2-sequestered. Considering the low cost, simplicity, and gigaton-scale sequestration potential, we believe that DAC based on alkaline industrial residue carbonation can be considered a “low-hanging fruit” in the pursuit of negative emissions to combat climate change.