In this study, hydrophobic nanochitin aerogels are synthesized via one-pot synthesis strategy and subsequent freeze-drying technique, employing nanochitin, hexanal and formaldehyde as primary components. The tert-butyl alcohol (TBA)/water binary solvents are found efficient for well mixing of hydrophilic nanochitin and hydrophobic hexanal, which is fundamental for fabricating hydrophobic aerogels with water contact angle as high as 105°. Schiff base reaction between amino groups in nanochitin and aldehyde groups in hexanal is believed to be the main reason for the successful hydrophobization of nanochitin aerogels. Additionally, formaldehyde is employed to enhance the mechanical properties of aerogels via ice templated crosslinking technique. Nanochitin aerogels prepared in this work possess surface area as high as 237 m2 g−1, which are believed benefiting from the TBA/water binary solvents with lower density, smaller ice crystal and convenience in freeze-drying. The ultralow density, ultrahigh porosity, and hydrophobicity nature also lead to the advanced oil adsorption (as high as 210 g g−1) of nanochitin aerogels. The simple preparation process, nature sustainability and excellent adsorption performance is believed rendering nanochitin aerogels as a viable alternative for the remediation of oil spills.