Soil carbon (SC) is important for food security, ecosystem functioning, and environmental health, especially in light of global climate change. The physico-chemical character of biochar (pyrolyzed crop residue) has been shown to augment SC levels. This review systematically compares the environmental and economic benefits of applying crop residue versus biochar produced from crop residues to soils and the potential implications for SC sequestration. Crop residues enhance the mineralization rate of SC, while biochar can increase or decrease SC depending on the types of biochar/soil and duration. Therefore, converting crop residues to biochar may be more efficient for sequestering SC, but may/may not be more cost-effective. In this review, special emphasis is given to understanding the underlying mechanisms and biogeochemical processes of biochar production, in particular: surface (crystallinity), redox, and ability to control electron transfer reactions. By using meta-analytics, we determined the role of biochar compared to crop residue to enhance the status of organic SC.