Abstract: Miscanthus-based lignocellulosic nanofibrils(LCNF) was produced by using citric acid pretreatment followed by the high-pressure homogenization with using miscanthus straw fiber as raw material. LCNF was cross-linked with 4, 4'-diphenyl-methane-diisocyanant(MDI) by using triethylamine as catalyst to obtain aerogel with high oil absorption capacity. The properties of aerogels were characterized by cold field emission scanning electron microscope, Fourier transform infrared spectrometer(FT-IR), thermogravimetric analyzer, and optical contact angle analyzer, and the oil absorption performance of aerogel was determined by gravimetric method. The results showed that the modified LCNF aerogel exhibited obvious multi-level rough micro/nanostructure with good thermal stability, hydrophobicity, and oil absorption capacity; the maximum weight loss temperature and water contact angle were 353.6℃ and 152.2°, respectively. FT-IR showed that cross-linking reaction was occurred between the hydroxylgroup on LCNF and the isocyanate group of MDI. When the mass ratio of LCNF to MDI was 1:4, the water contact angle of themodified aerogel was 138.1°, and the oil absorption performance was the bestwith chloroform absorption capacity of 41.6 g/g.