Biomass pyrolysis and the valorization of co-products (biochar, bio-oil, syngas) could be a sustainable management solution for agricultural and forest residues. Depending on its properties, biochar amended to soil could improve fertility. Moreover, biochar is expected to mitigate climate change by reducing soil greenhouse gas emissions, if its C/N ratio is lower than 30, and sequestrating carbon if its O/Corg and H/Corg ratios are lower than 0.2 and 0.7, respectively. However, the yield and properties of biochar are influenced by biomass feedstock and pyrolysis operating parameters. The objective of this research study was to validate an approach based on the response surface methodology, to identify the optimal pyrolysis operating parameters (temperature, solid residence time, and carrier gas flowrate), in order to produce engineered biochars for carbon sequestration. The pyrolysis of forest residues, switchgrass, and the solid fraction of pig manure, was carried out in a vertical auger reactor following a Box-Behnken design, in order to develop response surface models. The optimal pyrolysis operating parameters were estimated to obtain biochar with the lowest H/Corg and O/Corg ratios. Validation pyrolysis experiments confirmed that the selected approach can be used to accurately predict the optimal operating parameters for producing biochar with the desired properties to sequester carbon.