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Carbon is sequestered in soils by accumulation of recalcitrant organic matter and by bicarbonate weathering of silicate minerals. Carbon fixation by ecosystems helps drive weathering processes in soils and that in turn diverts carbon from annual photosynthesis-soil respiration cycling into the long-term geological carbon cycle. To quantify rates of carbon transfer during soil development in moist temperate grassland and desert scrubland ecosystems, we measured organic and inorganic residues derived from the interaction of soil biota and silicate mineral weathering for twenty-two soil profiles in arkosic sediments of differing ages. In moist temperate grasslands, net annual removal of carbon from the atmosphere by organic carbon accumulation and silicate weathering ranges from about 8.5 g m-2 yr-1 for young soils to 0.7 g m-2 yr-1 for old soils. In desert scrublands, net annual carbon removal is about 0.2 g m-2 yr-1 for young soils and 0.01 g m-2 yr-1 for old soils. In soils of both ecosystems, organic carbon accumulation exceeds CO2 removal by weathering, however, as soils age, rates of CO2 consumption by weathering accounts for greater amounts of carbon sequestration, increasing from 2% to 8% in the grassland soils and from 2% to 40% in the scrubland soils. In soils of desert scrublands, carbonate accumulation far outstrips organic carbon accumulation, but about 90% of this mass is derived from aerosolic sources that do not contribute to long-term sequestration of atmospheric carbon dioxide.