The formation of structured porous aerogels of nanofibrillated cellulose (NFC) by freeze-drying has been demonstrated. The aerogels have a high porosity, as shown by FE-SEM and nitrogen adsorption/desorption measurements, and a very low density ( < 0.03 g cm(-3)). The density and surface texture of the aerogels can be tuned by selecting the concentration of the NFC dispersions before freeze-drying. Chemical vapor deposition (CVD) of 1H, 1H, 2H, 2H-perfluorodecyltrichlorosilane (PFOTS) was used to uniformly coat the aerogel to tune their wetting properties towards non-polar liquids. An XPS analysis of the chemical composition of the PFOTS-modified aerogels demonstrated the reproducibility of the PFOTS-coating and the high atomic fluorine concentration (ca. 51%) in the surfaces. The modified aerogels formed a robust composite interface with high apparent contact angles (theta* >> 90 degrees) for castor oil (gamma(1v) = 35.8 mN m(-1)) and hexadecane (gamma(1v) = 27.5 mN m(-1)).