AbstractCustomizable 3D‐printed biopolymer hydrogels, highly sought after for diabetic wound management, face challenges in clinical application due to weak physical crosslinking within their constituent inks. In this study, a novel chitosan‐based hydrogel ink with a dense yet reversible physical crosslinking network is subtly designed for the rapid in situ fabrication of personalized diabetic wound dressing. This robust network is established through multiple electrostatic and hydrogen bonding interactions between unique carboxymethyl chitosan and nanoclay, further reinforced by the introduction of amide bonds, which act as double hydrogen bond donors/acceptors. Benefiting from this network, the ink with low nanoclay content exhibits remarkable self‐supporting properties, enabling high‐fidelity, large‐scale, and complex 3D printability without additional processing, while substantially retaining its inherent rheological properties after autoclave sterilization and the incorporation of active components. Given these advantages, this multifunctional 3D printable hydrogel can be rapidly in situ constructed on diabetic wounds. Simultaneously, the 3D‐printed hydrogel demonstrates biodegradability, anti‐swelling, and appropriate mechanical properties, along with remarkable in vitro antibacterial and pro‐angiogenic capabilities, leading to effective diabetic wound healing in vivo. This work offers a new strategy for creating highly self‐supporting biopolymer inks and paves the way for developing advanced personalized wound dressings.
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