Carbonate formation in waste from the steel industry could constitute a nontrivial proportion of the global requirements for removing carbon dioxide from the atmosphere at a potentially low cost. To utilize this potential, we examined atmospheric carbon dioxide sequestration in a >20 million ton legacy slag deposit in northern England, United Kingdom. Carbonates formed from the drainage water of the heap had stable carbon and oxygen isotope values between -12 and -25 ‰ and -5 and -18 ‰ for δ13C and δ18O, respectively, suggesting atmospheric carbon dioxide sequestration in high-pH solutions. From the analyses of solution saturation states, we estimate that between 280 and 2900 tons of CO2 have precipitated from the drainage waters. However, by combining a 37 year long data set of the drainage water chemistry with geospatial analysis, we estimate that <1% of the maximum carbon-capture potential of the deposit may have been realized. This implies that uncontrolled deposition of slag is insufficient to maximize carbon sequestration, and there may be considerable quantities of unreacted legacy deposits available for atmospheric carbon sequestration.