A very low-density oil-absorbing hydrophobic material was fabricated from cellulose nanofiber aerogels–coated silane substances. Nanocellulose aerogels (NCA) superabsorbents were prepared by freeze drying cellulose nanofibril dispersions at 0.2%, 0.5%, 0.8%, 1.0%, and 1.5% w/w. The NCA were hydrophobically modified with methyltrimethoxysilane. The surface morphology and wettability were characterized by scanning electron microscopy and static contact angle. The aerogels displayed an ultralow density (2.0–16.7 mg·cm-3), high porosity (99.9%–98.9%), and superhydrophobicity as evidenced by the contact angle of ~150° that enabled the aerogels to effectively absorb oil from an oil/water mixture. The absorption capacities of hydrophobic nanocellulose aerogels for waste engine oil and olive oil could be up to 140 g·g-1 and 179.1 g·g-1, respectively.