Cellulose acetate (CA) fibers were electrospun on a mesh template to create specific surface and pore structures for membrane applications. The mesh template CA fiber mats were impregnated with cellulose nanocrystals at varying weight percentages. The membranes showed nanotextured surfaces and improved mechanical properties post impregnation. More importantly, the hydrophilicity of the original CA fibers was increased from a hydrophobic contact angle of 102°–0° thereby creating an anti-fouling membrane surface structure. The membranes showed rejection of 20–56% for particles of 0.5–2.0 μm, indicating potential of these membranes in rejecting microorganisms from water. Furthermore, high rejection of dyes (80–99%) by adsorption and potential application as highly functional affinity membranes was demonstrated. These membranes can therefore be utilized as all-cellulose, green, scalable and low cost high flux membranes (> 20,000 LMH) for water cleaning applications in food industry where microorganisms and charged contaminants are to be removed.