Wound management remains a major concern in clinical care. Conventional dressings and hydrogels delivering drugs or cells can drive wound healing. However, these approaches are limited either by unnecessary bleeding and tissue tearing, or sophisticated fabrication, high cost, and drug-related side effects. Herein, a novel bioinspired glycopeptide hydrogel is rationally designed to mimic the glycoprotein components and nanofibrous architecture of cutaneous extracellular matrix (ECM) for self-accelerating the wound healing by regulating macrophage polarization without any additional therapeutic agents. The glycopeptide hydrogel, termed as GM-peptide hybrid hydrogel (GP gel), is established by the self-assembly of β-sheet Q11 peptide-grafted glucomannan, with nanofibrous structure, high water content, porosity, and self-healing properties. It is observed that GP gel displays remarkable capability of polarizing primary macrophages to M2-type phenotype in vitro and in vivo by inducing the activation of mannose receptors through ERK/STAT6 pathway. GP gel unprecedentedly expedites the wound closure rate and the regeneration of epidermis tissues in full-thickness skin excision models without drugs, exogenous cytokines, or seeded cells. More significantly, GP gel could promote angiogenesis in the repaired skin tissues. Collectively, such a novel ECM-mimicking glycopeptide hydrogel provides a highly effective treatment approach for skin wounds and may serve as a promising scaffold in regenerative medicine.

The treatment of difficult-to-heal wounds remains a substantial clinical challenge due to deteriorative tissue microenvironment including the loss of extracellular matrix (ECM), excessive inflammation, impaired angiogenesis, and bacterial infection. Inspired by the chemical components, fibrous structure, and biological function of natural ECM, antibacterial and tissue environment–responsive glycopeptide hybrid hydrogel was developed for chronic wound healing. The hydrogel can facilitate the cell proliferation and macrophage polarization to M2 phenotype, and show potent antibacterial efficacy against both Gram-negative and Gram-positive bacteria. Significantly, the glycopeptide hydrogel accelerated the reconstruction of methicillin-resistant Staphylococcus aureus (MRSA)–infected full-thickness diabetic and scalding skin by orchestrating a pro-regenerative response indicated by abundant M2-type macrophages, attenuated inflammation, and promoted angiogenesis. Collectively, ECM-mimetic and immunomodulatory glycopeptide hydrogel is a promising multifunctional dressing to reshape the damaged tissue environment without additional drugs, exogenous cytokines, or cells, providing an effective strategy for the repair and regeneration of chronic cutaneous wounds.

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Developing multifunctional wound dressings, possessing not only skin-like mechanical properties and adaptability, long-lasting moisture, and temperature tolerance that maximally mimics the human skin but also on-demand adhesion without unnecessary bleeding and secondary damage upon peeling, is necessary but remains a challenge. Herein, a novel dual cross-linked and multifunctional hydrogel, termed PSNC hydrogel for polymerized sulfobetaine methacrylate (SBMA), N-(2-amino-2oxyethyl)acrylamide (NAGA), and 1-carboxy-N-methyl-N-di(2methacryloyloxy-ethyl)methanaminium inner salt (CBMAX), was fabricated as a wound dressing for burn injuries via one-pot radical polymerization in glycerine (GLY)/H 2 O solvent. The dual crosslinked network of the PSNC hydrogel combined the double hydrogen bonding of N-(2-amino-2-oxyethyl)acrylamide (NAGA) with a covalently cross-linked zwitterionic network, endowing the hydrogel with skin−like mechanical properties with a high stretchability of 1613.8 ± 79.8%, a tensile strength of 77.5 ± 1.8 kPa, and a tensile modulus of 1.9 ± 0.1 kPa. Moreover, the hydrogel with well-developed adaptability can withstand skin deformation without breaking or debonding attributed to its good tissue adhesiveness and self-healing ability. Further, the utilization of the GLY/H 2 O binary solvent effectively prevented the crystallization and evaporation of free water, endowing the hydrogel with not only longlasting moisture but also excellent temperature tolerance in a wide range from −20 to 60 °C. More importantly, the PSNC hydrogel could effectively accelerate wound healing of burn injuries and could be easily removed on-demand with saline without causing secondary damage due to intense hydration. Such a novel PSNC zwitterionic hydrogel could be a promising candidate for the treatment of burn wounds and tissue regeneration.

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