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Despite the advantages of membrane processes, their high energy requirement remains a major challenge. Fabrication of nanocomposite membranes by incorporating various nanomaterials in the polymer matrix has shown promise for enhancing membrane flux. In this study, we embed functionalized cellulose nanofibers (CNFs) with high aspect ratios in the polymer matrix to create hydrophilic nanochannels that reduce membrane resistance and facilitate the facile transport of water molecules through the membrane. The results showed that the incorporation of 0.1 wt % CNF into the polymer matrix did not change the membrane flux (~15 L · m − 2 · h − 1 ) and Bovine Serum Albumin (BSA) Fraction V rejection, while increasing the CNF content to 0.3 wt % significantly enhanced the flux by seven times to ~100 L · m − 2 · h − 1 , but the rejection was decreased to 60–70%. Such a change in membrane performance was due to the formation of hydrophilic nanochannels by the incorporation of CNF (corroborated by the SEM images), decreasing the membrane resistance, and thus enhancing the flux. When the concentration of the CNF in the membrane matrix was further increased to 0.6 wt %, no further increase in the membrane flux was observed, however, the BSA rejection was found to increase to 85%. Such an increase in the rejection was related to the electrostatic repulsion between the negatively-charged CNF-loaded nanochannels and the BSA, as demonstrated by zeta potential measurements. SEM images showed the bridging effect of the CNF in the nanochannels with high CNF contents.