In order to solve the environmental problems caused by greenhouse gas emissions, cellulosenanofiber (CNF)/polyvinyl alcohol (PVA)/graphene oxide (GO) aerogel was obtained by step-by-step heating, tert-butanol replacement, freeze-drying, and high-temperature activation in this paper. The micromorphology, specific surface area, pore size distribution, and thermal stability of the prepared aerogels were analyzed by scanning electron microscopy, automatic surface area and porosity analysis, and thermo-gravimetric analysis. The interaction state and adsorption mechanism of CO2 and aerogel physical adsorption were described by Materials Studio simulation. The results showed that the adsorption process conformed to the Langmuir adsorption isotherm. After carbonization, the thermal stability of the aerogel was good (mass loss rate <1%). With the increase of GO content, its specific surface area increased (392.41 m2/g) and CO2 adsorption capacity increased (432.76 cm3/g at 273 K). The simulation results show that hydrogen bond energy and van der Waals adsorption are the main factors that help in adsorption of CO2 on the surface aerogel, and electrostatic adsorption is the secondary adsorption factor. The application of green material carbon-based aerogels is also in line with the concept of sustainable development.