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Cellulose nanofibrils are nano-scale materials with a diameter of several tens of nanometers. Cellulose nanofibrils' excellent mechanical and barrier properties make them attractive materials in the packaging industry. The morphology and crystallinity of obtained nano-cellulose greatly depend on the raw materials and the nano-fibrilization process. In this study, we investigated the effect of morphology and crystal structure of cellulose nanofibrils on coating performance, transparency, and barrier properties. Cellulose nanofibrils with a narrow diameter, high crystallinity and negative ion were fabricated as the concentration of the sulfuric acid was increased. As a result, post-treated cellulose nanofibrils could be easily coated due to narrow diameter and introduction of negative ion, and enhance oxygen barrier properties via the densely interconnected nanofiber surface.