This paper proposes enhancing CO2 sequestration and recovering degraded areas using Technosols constructed with coal waste and strategic materials. The evaluation of carbon capture considered four methods: (i) plant dry mass produced by Megathyrsus Maximus cv. Mombasa (ii) carbon incorporation via biochar, (iii) microbial biomass carbon, and (iv) mineral sequestration by lime. Local soil from the mine site was used as a control. Results show soil fertility parameters of the Technosols according to Brazilian guidelines. Plant growth increased with biochar incorporation but was still lower than in control soil. The pH, chemical, and mineralogical composition data were combined with geochemical reactions, showing the interaction of coal waste compounds, mainly pyrite with lime. Regarding calculating the CO2 capture potential, biochar and mineral carbonation were the most relevant means for the designed system. The best performance obtained can capture approximately 65 t CO2eq ha−1, about four times greater than the systems traditionally used to recover waste disposal areas. The study demonstrates the feasibility of incorporating mining site recovery, waste disposal, and emissions mitigation in a closed system, providing sustainable options for the coal mining industry.