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Managing soil to sequester C can help mitigate increasing CO2 in the atmosphere. To maximize this ecosystem service, more knowledge of factors influencing C sequestration is needed. The objectives of this study were to (i) quantify recovery of the roots, microbial biomass and composition, and soil structure across a chronosequence of grassland restorations and (ii) use a structural equation model to develop a data-based hypothesis on the relative influence of physical and biological soil properties on the soil C aggregate fraction diagnostic of sequestered C.