Agricultural lands under food and bio-energy crops, managed grass and permanent crops including agro-forestry, occupy about 40-50% of the Earth's land surface^1^. In 2005, agriculture accounted for an estimated emission of 5.1 to 6.1 GtCO2-eq/yr (10-12% of total global anthropogenic emissions of greenhouse gases (GHGs))^1^. However, measures to mitigate GHGs emission from agricultural soils are limited to improved cropland practices such as crop rotation, nutrient management, tillage/residue management, agroforestry, and return to natural vegetation^2^. These practices are not only far from substantially reducing GHGs emissions from soils or permanentlystabilizing soil organic matter^1-4^, but are also predicted to hardly match more than amaximum of 25% of the GHGs reductions required by the Kyoto Protocol within 2050^5^.Despite the knowledge that GHGs release from soil largely derives from biochemicaltransformations of plant litter and soil organic matter (SOM)^6-8^, no new and much wished biotechnological measures are adopted so far to augment mitigation^1^. Here we propose an innovative approach to mitigate GHGs emissions from soils based on the insitu photo-polymerization of SOM under biomimetic catalysis. Three Mediterranean soils of different physical and chemical properties were added with a synthetic watersolubleiron-porphyrin, irradiated by solar light, and subjected to 15, and 30 wetting and drying cycles. We found that the in situ catalysed photo-polymerization of SOM increased soil physical aggregation, shifted OC into larger soil aggregates, and reduced CO~2~ released by microbial respiration. Our findings suggest that "green" catalytic technologies can become viable soil management practices to enhance mitigation of GHGs emission from arable soils and contribute to match the expectations of the post-Kyoto Protocol in the agricultural sector