Magnetic superhydrophobic materials have broad application prospect in oil-water separation. In this study, a magnetic and superhydrophobic aerogel with lamellar structure was successfully prepared using cellulose nanofibrils (CNF) as the skeleton, Fe3O4 as the magnetic ion, 1H, 1H, 2H, 2H trialkylfluorooctane triethoxysilane (FS) and 3-(2-aminoethyl amino)-propyl trimethoxysilane (AS) as the combined modifier. The prepared aerogel shows lower density (38.63 mg/cm3), excellent magnetic (15.13 emu/g), high elasticity and good oil sorption properties (21 g/g). In addition, FS/AS also exhibits excellent mechanical properties and superhydrophobic ability (water contact angle (WCA) of 151.9 ± 1.4°), as it provides sufficient toughness and low surface energy for the layer-branch structure. It should be noted that the entire preparation process is carried out in the aqueous phase, without the use of any organic solvents, providing a green oil-water separation strategy.