The increase in waste generation from food processing and agricultural residues presents a significant challenge for sustainable development and waste management. Utilizing these biomass waste materials for valuable applications can help address this issue, while promoting a circular economy. In this context, the current study focuses on the valorization of waste materials of organic origin for CO 2 capture, a crucial component in global efforts to mitigate climate change and reduce the planet's warming. The investigated polymeric aerogels were synthesized using byproducts from food processing and agricultural residue waste products, specifically crustacean shells and sugarcane bagasse. A comprehensive set of analytical techniques, including viscometry, Fourier transform infrared spectroscopy (FTIR), energy dispersive X-ray spectroscopy (EDX), thermogravimetric analysis (TGA), X-ray diffraction (XRD), field emission scanning electron microscopy (FESEM), transmission electron microscopy (TEM), and Brunauer−Emmett−Teller (BET) surface area analysis, were employed to examine the physicochemical, thermal, microstructural, and textural properties of the prepared materials. These adsorbents demonstrated promising prospects for carbon dioxide capture, adsorbing up to 5.78 mg/g of the gas at 273 K and 2.82 mg/g at 298 K. Considering their sorption performance, the low cost of raw materials, and the potential for scaling up, this work further validates the adsorbent-based postcombustion carbon capture technology as an effective approach for addressing the detrimental consequences of carbon dioxide emissions.