Abstract
Hydroplastics with water-plasticizing effects and programmability are highly desired yet challenges arise from assembling renewable cellulose into hydroplastics with reversible adhesion and enhanced mechanical performance through water-enhancement effects. Here, inspired by zippers, the issue that water molecules are difficult to enhance the comprehensive performances of hydroplastics is addressed by regulating molecular-scale polarity using thioctic acid (TA), combined with reconfigured molecular network under imbalanced polarity environment created by water. This approach enables the fabrication of transparent cellulose hydroplastics (91%) with mechanical performance that can be enhanced to 203 MPa under hydration-dehydration cycles, surpass most cellulose hydroplastics. Moreover, unlike conventional cellulose hydroplastics, the hydroplastic exhibits excellent water-induced reversible adhesion (up to 37 MPa) and rapid programmability (5 minutes). These unique performance advantages open a unique avenue for cellulose to prepare high-performance multifunctional hydroplastics from top-down, dedicated to replacing traditional plastics and reducing the consumption of petrochemical resources.
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All data that support the findings of this study are available within the paper and its supplementary information files or are available from the corresponding authors upon request. Source data are provided with this paper.
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Acknowledgements
This work was supported by the National Natural Science Key Foundation of China (52273095, H.-Y.Y.), the Outstanding Youth Project of Zhejiang Provincial Natural Science Foundation (LR22E030002, H.-Y.Y.), and the Key Research and Development Program of Zhejiang Province (Grant No. 2024C03224; 2026C02A1066, H.-Y.Y.).
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G.C. and H.-Y.Y. conceived and designed the idea. G.C., C.H., and H.-Y.Y. designed the experiments, collected and analyzed the data. G.C. papered the experiments and characterizations, analyzed DFT and MD calculations, discussed the results and prepared the manuscript, wrote the manuscript. G.C., C.H., Y.D., Y.Z., Y.C. and K.C.T. designed the experiment.
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Nature Communications thanks Tian Li, who co-reviewed with Xiwei Shan; Chaoji Chen and the other, anonymous, reviewer for their contribution to the peer review of this work. A peer review file is available
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Chen, G., Huang, C., Dong, Y. et al. Zipper-inspired molecular polarity strategy enabling robust adhesive hydroplastics as sustainable plastic substitutes. Nat Commun (2026). https://doi.org/10.1038/s41467-026-70998-9
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DOI: https://doi.org/10.1038/s41467-026-70998-9
