Abstract: Due to the high porosity and high absorption characteristics, aerogel has been a promising candidate material in the field of oily wastewater treatment. However, the reported aerogels were still suffering from insufficient mechanical strength, complicated fabrication process and high preparation cost, which limited the application of aerogels in the field of oil-water separation. Bentonite (BT) has the characteristics of low price, abundant source and excellent mechanical properties, which can effectively improve the mechanical properties of aerogels. In this paper, hydrophobic nanocellulose-chitosan/exfoliated bentonite aerogels (CNC/BTex) were synthesized by introducing exfoliated bentonite (BTex) onto a cross-linked network of carboxycellulose nanofibres (CNF-C) and chitosan (CS) by a simple freeze-drying and ambient temperature impregnation method. The prepared CNC/BTex aerogel exhibited excellent hydrophobic properties (water contact angle 133°), recovered deformation within 5 s after extrusion and showed good mechanical properties. The adsorption capacities for different oils (hexane, cyclohexane, dichloromethane, cooking oil and engine oil) ranged from 18.48-40.20 g·g⁻¹. Using dichloromethane and cyclohexane as the main research objects, the oil adsorption performance remained stable (90% of the original adsorption capacity) after five cycles of use. In summary, the present work provides a reference for the preparation of low-cost and high-performance adsorbent materials for oil-water separation.