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In this study,cellulose nanofibrils (CNF) of high charge (H-P-CNF) and screened size (H-P-CNF-S) were fabricated by increasing the charge of phosphorylated cellulose nanofibrils (P-CNFs) during the pre-treatment step of CNF production.Results show that the H-P-CNF have a significantly higher charge (3.41 mmol g-1) compared with P-CNF (1.86 mmol g-1).Centrifugation of H-P-CNF gave a supernatant with higher charge (5.4 mmol g-1) and a reduced size (H-P-CNF-S).These tailored nanocelluloses were added to polyvinyl alcohol (PVA) solutions and the suspensions were successfully coated on porous polysulfone (PSf) supports to produce thin-film nanocomposite membranes.The humid mixed gas permeation tests show that CO2 permeability increases for membranes with the addition of H-P-CNF-S by 52% and 160%,compared with the P-CNF/PVA membrane and neat PVA membrane,respectively.