AbstractThe study of different natural carbon sinks has become especially important because of climate change effects. The restoration of contaminated areas can be an ideal strategy for carbon sequestration. The studied area was affected by toxic Aznalcóllar mine spill in 1998. Restoration process of the contaminated area was based, mainly, on the use of two organic amendments: leonardite (LE) and biosolid compost (BC). The objective of this study was to verify whether the application of these amendments promotes the long‐term carbon sequestration in this soil. Five treatments were established: untreated control, biosolid compost (doses 4 and 2) and leonardite (doses 4 and 2). The addition of amendments implied an improvement in soil quality that was directly related to the amendment dose: decrease in bulk density, increase in pH, higher respiration rates and an improvement in the stratification ratio. Dose‐dependent changes in the molecular composition of soil organic matter were shown by nuclear magnetic resonance analysis. Both amendments promoted carbon retention, although because of the low mineralization rates of soil organic matter in LE treatments, the carbon storage was higher. The dosage effect on the carbon balance was more important in LE treatments, whereas in the BC treatments, the balance was similar for both doses. Our findings suggest that LE4 significantly increased the total organic carbon and it was the most suitable treatment for long‐term carbon storage, because of its molecular composition rich in relatively stable aromatic and lignin‐derived compounds. Copyright © 2015 John Wiley & Sons, Ltd.