As an environmentally friendly aerogel with outstanding performances, the improvement of mechanical properties is urgently required for cellulose aerogel development. In this study, a cellulose aerogel with good mechanical properties was successfully fabricated using nanocrystalline cellulose (NCC) as reinforcer. Characterization results demonstrated that NCC was embedded well into the cellulose aerogel. Tests and evaluation showed that the compressive modulus of the NCC reinforced cellulose aerogel was significantly improved, about 6 times higher than that of the pure cellulose aerogel.Furthermore, after modification with trimethylchlorosilane via a cold plasma treatment, the NCC reinforced aerogel became hydrophobic but its oleophilic property remained. This aerogel showed good adsorption capacity, reached saturation rapidly and possessed good reusability. Reinforced mechanical properties with NCC make this cellulose aerogel a very promising material for highly efficient separation and extraction of organic pollutants and oils from water.