Carbon aerogel is a promising material in various applications, such as water treatment, insulators, catalysts, and sensors, due to its porosity, low density, conductivity, and good chemical stability. In this study, an inexpensive carbon aerogel was prepared through lyophilization and post-pyrolysis using waste paper. However, carbon aerogel, in the form of short belts, is randomly entangled without a crosslinking agent and has weak mechanical properties, thus limiting its applications, which would otherwise be various. In this paper, a novel strategy is proposed to fabricate a PDMS-coated carbon aerogel (Aerogel@PDMS). Benefiting from microwave heating, precise PDMS coating onto the carbon frame was able to be carried out in a short amount of time. PDMS coating firmly tied the carbon microstructure, maintaining a unique aerogel property without blocking its porous structure. FE-SEM, RAMAN, XPS, and FT-IR were all used to confirm the surface change in PDMS coating. Compressible stability and water contact angle measurement showed that Aerogel@PDMS is a perspective organic solvent absorbent due to its good resilience and its hydrophobicity, and, as a result, its organic solvent absorption capacity and repeated absorption were evaluated, ultimately suggesting a promising material in oil clean-up and pollution remediation in water. Based on our experimental results, we identified elastic carbon aerogels provided by a novel coating technology. In the future, then, the developed carbon/PDMS composite can be examined as a promising option for various applications, such as environmental sensors, virus sensors, and wearable sensors.