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Hydrogels showing strong adhesion to different substrates have garnered significant attention for engineering applications. However, the current development of such hydrogel-based adhesive is predominantly limited to synthetic polymers, owing to their exceptional performance and an extensive array of chemical options. To advance the development of sustainable hydrogel-based adhesives, we successfully create a highly robust all-cellulose hydrogel-based adhesive, which is composed of concentrated dialcohol cellulose nanorods (DCNRs) and relies on enhanced hydrogen bonding interactions between cellulose and the substrate. We implement a sequential oxidization-reduction process to achieve this high-performance all-cellulose hydrogel, which is realized by converting the two secondary hydroxyl groups within an anhydroglucose unit into two primary hydroxyl groups, while simultaneously linearizing the cellulose chains. Such structural and chemical modifications on cellulose chains increase out-of-plane interactions between the DCNRs hydrogel and substrate, as simulations indicate. Additionally, these modifications enhance the flexibility of the cellulose chains, which would otherwise be rigid. The resulting all-cellulose hydrogels demonstrate injectability and strong adhesion capability to a wide range of substrates, including wood, metal, glass, and plastic. This green and sustainable all-cellulose hydrogel-based adhesive holds great promise for future bio-based adhesive design.