In this article, we report a new sustainable synthesis procedure for manufacturing chitosan/silica CO2 adsorbents. Chitosan is a naturally abundant material and contains amine functionality, which is essential for selective CO2 adsorptions. It is, therefore, ideally suited for manufacturing CO2 adsorbents on a large scale. By coating chitosan onto high‐surface‐area mesoporous silica supports, including commercial fumed silica (an economical and accessible reagent) and synthetic SBA‐15 and MCF silicas, we have prepared a new family of CO2 adsorbents, which have been fully characterised with nitrogen adsorption isotherms, thermogravimetric analysis/differential scanning calorimetry, TEM, FTIR spectroscopy and Raman spectroscopy. These adsorbents have achieved a significant CO2 adsorption capacity of up to 0.98 mmol g−1 at ambient conditions (P=1 atm and T=25 °C). The materials can also be fully regenerated/recycled on demand at temperatures as low as 75 °C with a >85 % retention of the adsorption capacity after 4 cycles, which makes them promising candidates for advanced CO2 capture, storage and utilisation technology. It captures the carbon: Chitosan‐coated mesoporous silica materials have been prepared as a new family of CO2 adsorbents. These adsorbents have achieved a significant CO2 adsorption capacity of up to 0.98 mmol g−1 at P=1 atm and T=25 °C, and they can also be fully regenerated/recycled at temperatures as low as 75 °C.