Adsorbent materials with high absorption capacity, stable mechanical properties, greenness and economy are highly desirable for efficient removal and recovery of oil from wastewater. Herein, an ultralight, low-cost and reusable hydrophobic aerogel of cellulose acetate/polyethylene oxide hybrid nanofibers was developed through thermal crosslinking and organosilicon modification. Through thermal crosslinking and an ice crystal template, a hierarchical pore structure was obtained which endowed the aerogel with mechanical stability and oil-absorption capacity. In addition, the structure was further strengthened after chemical vapor deposition of methyl trichlorosilane and good hydrophobicity (contact angle of 135.5°) can be realized. The surface-modified aerogel presented an ultralow density (8.74 mg cm−3), excellent resilience (completely recover to its original height after 50 compression cycles), high absorption capacity (weight gain of 63–128 g g−1) and reusability. Therefore, nanofibrous aerogels with outstanding compressive resilience and reusability make it promising to meet the increasing demand in the field of oil pollution cleaning.
