Hydrophobic organic pollutants in industrial wastewater and oil spillage have attracted wide attention. It is thus important to develop a variety of adsorbents like activated carbon, biochar, zeolite, graphene, etc.. However, carbon-based porous materials exhibit poor thermal stability and flammability, having secure risks during high-temperature applications and thermal regeneration processes. Silicon-based porous materials like zeolite are complex to prepare and difficult to effectively remove multiple organic pollutants simultaneously. Montmorillonite-based adsorbents become popular due to their low cost and environmental friendliness. However, montmorillonite as a powder has challenges in practical applications such as clogging, leakage, and recovery difficulties. It is thus effective in converting montmorillonite into fixed-form aerogel materials.Polyurethane sponge (PU) as an ideal substrate for developing porous aerogels can enhance the mechanical properties of the adsorbents due to its biodegradability, affordability, low density, and customizable dimensions. In this paper, low-density,recyclable, and cost-effective organic montmorillonite/polyurethane sponge composite aerogels were prepared via ultrasonic swelling and freeze-drying. The composite aerogel was evaluated for its adsorption/absorption capabilities towards benzene,bisphenol A, nitrobenzene, oils, and organic solvents. In addition, the reusability and flammability characteristics of the aerogel were also analyzed.