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The cellulose nanocrystals (CNC) has attracted widespread attention in reinforced materials. However, the application of CNC in electrospinning has been limited due to its self-polymerization. Herein, a cobweb-like nanofibrous membrane was fabricated by electrospinning the polyacrylonitrile (PAN) and sulfydryl-functionalized CNC (SC). The SC content could reach to 48 wt% after the thiolation modification. The membrane with ultrafine fibers and interlaced nets possessed outstanding porosity (91.7%) and underwater superoleophobicity. An