The energy-intensive and time-consuming process required for disassembling natural materials into nanoblocks are the major obstacles for the practical applications of biopolymer nanomaterials. Herein, a one-pot, energy-efficient and directional preparation method for gently exfoliating cellulose into nanosheets was achieved by surface modification assisted swelling process. The resulting cellulose nanosheets (CNSs) exhibited diameters ranging from 100 to 480 nm and thicknesses of approximately 5 nm, with a maximum yield of 97.9 %. This method could be widely applicable to common cellulose raw materials. Contrary to other nanocellulose reported previously, CNSs could be dried and stored in solid state, and re-dispersed in aqueous phase, thereby convenient for storage and transportation. Cellulose nanosheets films (CNSFs) obtained from CNSs showed high transparencies (>90 %) and excellent gas barrier properties, especially for the water vapor permeability of only 0.0072×10−10 cm3 cm cm−2 s−1 Pa−1, which were superior to other cellulose based films. In the simulation experiment of dry food packaging, CNSF10 possessed remarkable water vapor and oxygen blocking capabilities comparable to commercial cling films and met the practical requirements. The preparing process of CNSs reported here had the advantages including easy implementation, energy efficiency, and environmentally friendliness, and expanded possibilities for large-scale and widespread utilization of nanocellulose.
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