Carbon dioxide (CO2) is one of the main greenhouse gases that contribute to global warming. CO2 capture technology is urgently needed to mitigate its impact on society and ecosystems. Researchers use cellulose-based materials to adsorb CO2, exploring its potential in gas separation and capture. This study centered its efforts on advancing the development of cellulose aerogels capable of synergistically adsorbing CO2 by utilizing amino groups and metal–organic frameworks. Cellulose aerogels were prepared by incorporating epichlorohydrin as a cross-linking agent along with metal–organic frameworks and functionalized polyethyleneimine. The nitrogen adsorption–desorption isotherms were tested at 77 K and 1 bar, and the sample exhibited typical adsorption curves of mesoporous materials. The specific surface area of the sample underwent calculation using the Brunauer-Emmett-Teller (BET) equation, resulting in a specific surface area value of 153.1 m2/g, which represents a 230 % increase compared to the pre-modification state. At 298 K and 1 bar, it can adsorb a maximum of 9.26 mmol/g of CO2. This study has established a new foundation for cellulose-based CO2 capture and contributes to the high-value utilization of bamboo resources.