Background: During de-pulping of açai (Euterpe oleracea) for juice production in the Amazonia, large amounts of fibrous waste are daily discarded, a promising substrate for production of high-value cellulose nanofibrils. Therefore, this study sought to evaluate the modifications of açai surface fibers submitted to chemical pretreatment steps and compare the quality of nanostructured films produced with different cycles of mechanical nanofibrillation. Results:A 2-hour pretreatment (at 5% of NaOH) followed by two NaOH/H 2 O 2 bleaching steps resulted in fibers with increased length and reduced diameter compared to raw fibers while preserving fiber integrity and cellulose I structure. The increase of fibers' grinding cycles from 3 (minimum to gel point) to 21 (maximum suspension thickness) resulted in nanofibril films with higher crystallinity properties, uniform thickness, compacted morphology, and smoother surface. Nanofibril films formed after different numbers of passages exhibited similar mechanical strength, but distinct barrier properties. Conclusion:Açaí waste films produced with fibers submitted to 3 grinding cycles can be recommended for packaging applications that demand easily dissolving, such as instantaneous food. Oppositely, açaí fibers subjected to 21 cycles in grinder provide films suitable for water-resistant packaging, ideal for secondary coatings of papers and paperboards.