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Carbonation of ultramafic mine tailings has the potential to offset greenhouse gas emissions from mining by trapping CO₂ within the crystal structures of Mg-carbonate minerals and hydrotalcite supergroup minerals, which form as weathering products in tailings storage facilities. Here, we present a detailed geochemical and mineralogical assessment of tailings from the Woodsreef Chrysotile Mine, New South Wales, Australia, demonstrating that coupling mineralogical and elemental datasets improves the accuracy of carbon accounting in mined landscapes. Detailed analysis of tailings mineralogy using quantitative X-ray diffraction (XRD) and total carbon analyses reveals that previous assessments of passive mineral carbonation at Woodsreef have been underestimated. Maximum values for the abundance of total carbon (up to 0.4 wt%), as well as the abundances of secondary carbonate minerals (i.e., up to 1.9 wt …