A facile and environmental-friendly approach was developed for the preparation of the cross-linked nanocellulose aerogel through the freeze-drying process and subsequent esterification. The as-prepared aerogel had a three-dimensional cellular microstructure with ultra-low density of 6.05 mg·cm⁻³ and high porosity (99.61%). After modifying by chemical vapor deposition (CVD) with hexadecyltrimethoxysilane (HTMS), the nanocellulose aerogel displayed stable super-hydrophobicity and super-oleophilicity with water contact angle of 151°, and had excellent adsorption performance for various oil and organic solvents with the adsorption capacity of 77~226 g/g. Even after 30 cycles, the adsorption capacity of the nanocellulose aerogel for chloroform was as high as 170 g/g, indicating its outstanding reusability. Therefore, the superhydrophobic cross-linked nanocellulose aerogel is a promising oil adsorbent for wastewater treatment.