Biochar has been extensively utilized to amend soil and mitigate greenhouse gas (GHG) emissions from croplands. However, the effectiveness of biochar application in reducing cropland GHG emissions remains uncertain due to variations in soil properties and environmental conditions across regions. In this study, the impact of biochar surface functional groups on soil GHG emissions was investigated using molecular model calculation. Machine learning (ML) technology was applied to predict the responses of soil GHG emissions and crop yields under different biochar feedstocks and application rates, aiming to determine the optimum biochar application strategies based on specific soil properties and environmental conditions on a global scale. The findings suggest that the functional groups play an essential role in determining biochar surface activity and the soil's capacity for adsorbing GHGs. ML was an effective method in predicting the changes in soil GHG emissions and crop yield following biochar application. Moreover, poor-fertility soils exhibited greater changes in GHG emissions compared to fertile soil. Implementing an optimized global strategy for biochar application may result in a substantial reduction of 684.25 Tg year-1 CO2 equivalent (equivalent to 7.87% of global cropland GHG emissions) while simultaneously improving crop yields. This study improves our understanding of the interaction between biochar surface properties and soil GHG, confirming the potential of global biochar application strategies in mitigating cropland GHG emissions and addressing global climate degradation. Further research efforts are required to optimize such strategies. An optimized biochar application strategy could effectively reduce global cropland GHG emissionsGA-BPNN-based ML excels at handling nonlinear responses of soil GHG emissions to biochar additionBiochar surface functional groups contribute to the decomposition of recalcitrant carbonPoor-fertility soil exhibited a greater response to biochar application compared to fertile soil