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Cellulose provides promising alternatives to synthetic plastics to achieve a low carbon footprint and biodegradable materials, which have significant positive impacts on environmental protection and on human health. In this work, sulfated holocellulose fibers and sulfated holocellulose nanofibrils (SHCNFs) are prepared using a combination of delignification with derivatization to achieve high fiber yield, superior recycling performance, and less energy consumption of the final products by means of preserving hemicellulose. Derivatization of the surface with sulfate groups provides a further means to avoid excessive aggregation between adjacent cellulose surfaces. Interestingly, hemicellulose increases the accessibility of holocellulose fibers and reduces the embodied energy during sulfate esterification. The presence of hemicellulose imparts high optical transmittance, mechanical performance (ultimate strength, 390 MPa; Young's modulus, 33 GPa), and recyclability for SHCNFs. This combination of two treatments can unlock the greater potential of cellulose as a sustainable material over its entire life cycle., (Copyright © 2022 Elsevier Ltd. All rights reserved.)