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Chronic nonhealing diabetic wound therapy and complete skin regeneration remains a critical clinical challenge. The controlled release of bioactive factors from a multifunctional hydrogel was a promising strategy to repair chronic wounds. Herein, for the first time, we developed an injectable, self-healing and antibacterial polypeptide-based FHE hydrogel (F127/OHA-EPL) with stimuli-responsive adipose-derived mesenchymal stem cells exosomes (AMSCs-exo) release for synergistically enhancing chronic wound healing and complete skin regeneration. The materials characterization, antibacterial activity, stimulated cellular behavior and full-thickness diabetic wound healing ability of the hydrogels were performed and analyzed. The FHE hydrogel possessed multifunctional properties including fast self-healing process, shear-thinning injectable ability, efficient antibacterial activity, and long term pH-responsive bioactive exosomes release behavior. , the FHE@exosomes (FHE@exo) hydrogel significantly promoted the proliferation, migration and tube formation ability of human umbilical vein endothelial cells (HUVECs). , the FHE@exo hydrogel significantly enhanced the healing efficiency of diabetic full-thickness cutaneous wounds, characterized with enhanced wound closure rates, fast angiogenesis, re-epithelization and collagen deposition within the wound site. Moreover, the FHE@exo hydrogel displayed better healing outcomes than those of exosomes or FHE hydrogel alone, suggesting that the sustained release of exosomes and FHE hydrogel can synergistically facilitate diabetic wound healing. Skin appendages and less scar tissue also appeared in FHE@exo hydrogel treated wounds, indicating its potent ability to achieve complete skin regeneration. This work offers a new approach for repairing chronic wounds completely through a multifunctional hydrogel with controlled exosomes release.

The fabrication of highly biocompatible hydrogels with multiple unique healing abilities for the whole healing process, for example, multifunctional hydrogels with injectable, degradation, antibacterial, antihypoxic, and wound healing–promoting properties that match the dynamic healing process of skin flap regeneration, is currently a research challenge. Here, a multifunctional and dynamic coordinative polyethylene glycol (PEG) hydrogel with mangiferin liposomes (MF‐Lip@PEG) is developed for clinical applications through Ag–S coordination of four‐arm‐PEG‐SH and Ag+. Compared to MF‐PEG, MF‐Lip@PEG exhibits self‐healing properties, lower swelling percentages, and a longer endurance period. Moreover, the hydrogel exhibits excellent drug dispersibility and release characteristics for slow and persistent drug delivery. In vitro studies show that the hydrogel is biocompatible and nontoxic to cells, and exerts an outstanding neovascularization‐promoting effect. The MF‐Lip@PEG also exhibits a strong cytoprotective effect against hypoxia‐induced apoptosis through regulation of the Bax/Bcl‐2/caspase‐3 pathway. In a random skin flap animal model, the MF‐Lip@PEG is injectable and convenient to deliver into the skin flap, providing excellent anti‐inflammation, anti‐infection, and proneovascularization effects and significantly reducing the skin flap necrosis rate. In general, the MF‐Lip@PEG possesses outstanding multifunctionality for the dynamic healing process of skin flap regeneration. A multifunctional and convenient dynamic coordinative polyethylene glycol (PEG) hydrogel with mangiferin liposomes is presented through Ag–S coordination of four‐arm‐PEG‐SH and Ag+ is fabricated for promoting skin flap regeneration via outstanding antihypoxia, anti‐inflammation, and neovascularization functions.

Traditional patches, such as sticking plaster or acrylic adhesives used for over a hundred years, lack functionality. To address this issue of poor functionality, adhesive hydrogel patches have emerged as an efficient bioactive multifunctional alternative. Hydrogels are three‐dimensional, water‐swellable, and polymeric materials closely resembling the native tissue architecture. The physicochemical properties of hydrogels can be modified easily, allowing them to be suitable for various biomedical applications. Moreover, adhesive properties can be imparted to hydrogels through physicochemical manipulations, making them ideal candidates for supplementing or replacing traditional sticking plaster. As a result, sticky hydrogel patches are widely used for transdermal drug delivery and have even found commercial purposes. Beyond transdermal delivery, such hydrogel patches have also found applications in cardiac therapy, cancer research, and biosensing, among other applications. In this mini‐review, we critically discuss the challenges of fabricating multifunctional adhesive hydrogel patches. Furthermore, we introduce some of the chemical strategies involved with fabricating the patches. We also review their emerging biomedical applications. Finally, we explore their potential future in the flourishing field of tissue engineering and drug delivery.

Factor-free biomaterial scaffolds play an increasingly important role in promoting bone reconstruction and regeneration. However, the complicated and variable pathophysiological microenvironments of the injury sites under diabetic conditions, including the vicious cycle of oxidative stress and inflammatory response, impaired osteo/angiogenesis function and hyperactive osteoclastogenesis, as well as increased susceptibility to bacterial infection, may largely weaken the therapeutic potential of implanted scaffolds, leading to uncontrolled and poor outcomes of bone defect healing. To tackle the aforementioned challenges, a mild photothermal-assisted multifunctional therapeutic platform (denoted as GAD/MC) that integrates copper-containing two-dimensional Ti C T MXene nanosheets, gelatin methacrylate, and alginate-graft-dopamine was proposed to achieve efficient and synergistic therapy for diabetic bone defects. Thereinto, copper-decorated MXene (MC) nanosheets were employed as both functional crosslinkers and nanofillers to participate in the construction of an interpenetrating polymer network structure through multiple covalent and noncovalent bonds, which conferred the hydrogel with advantageous traits like enhanced mechanical properties, injectability and moldability, strong bone tissue adhesion and self-healing ability, as well as excellent anti-swelling and near-infrared (NIR) photothermal conversion capabilities. On account of the NIR/pH dual-responsive properties, the resulting hydrogel system was capable of achieving the controlled and stimuli-responsive release of bioactive Cu , allowing on-demand delivery at the site of injury. Moreover, with the assistance of mild photothermal effects, this integrated hydrogel system demonstrated remarkable antibacterial and antioxidant properties. It effectively scavenged excessive reactive oxygen species (ROS), inhibited inflammatory responses, and promoted macrophage polarization towards the pro-healing M2 phenotype. Such characteristics were beneficial for recreating an optimized microenvironment that supported the adhesion, proliferation, migration, and differentiation of osteoblasts and endothelial cells, while concurrently inhibiting osteoclast function. In a critical-sized cranial defect model using diabetic rats, the injectable GAD/MC hydrogel system combined with on-demand mild hyperthermia further synergistically accelerated new bone formation and bone healing processes by eliminating intracellular ROS, ameliorating inflammation, orchestrating M2 macrophage polarization, promoting osteo/angiogenesis, and suppressing osteoclastogenesis. Overall, the constructed multifunctional injectable hydrogel system has emerged as a promising therapeutic candidate for addressing complex bone-related challenges by remodeling the disordered immune microenvironment and expediting the bone healing process.

Chitosan is a promising naturally derived polysaccharide to be used in hydrogel forms for pharmaceutical and biomedical applications. The multifunctional chitosan-based hydrogels have attractive properties such as the ability to encapsulate, carry, and release the drug, biocompatibility, biodegradability, and non-immunogenicity. In this review, the advanced functions of the chitosan-based hydrogels are summarized, with emphasis on fabrications and resultant properties reported in literature from the recent decade. The recent progress in the applications of drug delivery, tissue engineering, disease treatments, and biosensors are reviewed. Current challenges and future development direction of the chitosan-based hydrogels for pharmaceutical and biomedical applications are prospected.

Chronic inflammatory diseases, such as intervertebral disc degeneration (IVDD), which affect the lives of hundreds of millions of people, still lack effective and precise treatments. In this study, a novel hydrogel system with many extraordinary properties is developed for gene–cell combination therapy of IVDD. Phenylboronic acid‐modified G5 PAMAM (G5‐PBA) is first synthesized, and therapeutic siRNA silencing the expression of P65 mixed with G5‐PBA (siRNA@G5‐PBA) is then embedded into the hydrogel (siRNA@G5‐PBA@Gel) based on multi‐dynamic bonds including acyl hydrazone bonds, imine linkage, π–π stacking, and hydrogen bonding interactions. Local and acidic inflammatory microenvironment‐responsive gene‐drug release can achieve spatiotemporal regulation of gene expression. In addition, gene‐drug release from the hydrogel can be sustained for more than 28 days in vitro and in vivo, greatly inhibiting the secretion of inflammatory factors and the subsequent degeneration of nucleus pulposus (NP) cells induced by lipopolysaccharide (LPS). Through prolonged inhibition of the P65/NLRP3 signaling pathway, the siRNA@G5‐PBA@Gel is verified to relieve inflammatory storms, which can significantly enhance the regeneration of IVD when combined with cell therapy. Overall, this study proposes an innovative system for gene–cell combination therapy and a precise and minimally invasive treatment method for IVD regeneration. This work innovatively develops an injectable, self‐healing, adhesive, hemostatic, antibacterial, and biocompatible multifunctional hydrogel system for local and acidic inflammatory microenvironment‐responsive gene‐drug release and cell delivery, which is a precise and minimally invasive treatment method of IVDD and can achieve IVD regeneration through gene–cell combination therapy.

Periodontitis and myocardial infarction (MI), the leading cause of mortality worldwide, represent globally prevalent inflammatory diseases with bidirectional pathophysiological links. Despite the urgent demand for non-invasive strategies capable of alleviating local periodontal destruction while mitigating associated systemic cardiovascular complications, no integrated treatment modality currently exists. To address this challenge, a protein-loaded antibacterial hydrogel, thiolated chitosan/AMP-PEG-maleimide (C1.5P4/BMP-2), with novel sustained protein release properties was developed. This hydrogel features an interconnected microporous architecture that: (1) enables high-efficiency BMP-2 protein encapsulation, (2) preserves protein bioactivity while ensuring sustained release, thereby addressing the recognized challenge of hydrogel-based protein delivery, (3) confers potent antibacterial properties, (4) facilitates remote cardiac function improvement by resolving periodontal inflammation. In murine models, locally, it attenuated alveolar bone loss (2-fold greater bone regeneration vs controls) while systemically improving post-MI cardiac function (75.6% higher ejection fraction). Mechanistically, the hydrogel's protein-protective microenvironment synergized with its antimicrobial action selectively inhibiting Gram-negative (G−) anaerobic pathogens (primary periodontal culprits) while enriching Gram-positive (G+) commensals, regulating biofilm G−/G+ ratio. Concomitantly, this dual action modulates the oral-cardiac inflammatory axis, specifically downregulating B2 cell/TNF-α signaling to mitigate systemic inflammation associated with MI. Collectively, this study presents a novel non-invasive protein-stabilizing hydrogel that addresses periodontitis-MI comorbidity through sustained osteogenic factor delivery coupled with microbiome-immune modulation. Image 1 •The first dual-targeting hydrogel for periodontitis-MI comorbidity via a single periodontal injection.•High protein loading capacity with sustained bioactivity and tunable injectability for periodontal pockets.•Gram-negative selective antimicrobial and osteogenic synergy of the hydrogel for periodontitis.•Dual-organ healing ability of the hydrogel via mediating microbiome-immune crosstalk.

Gastrostomy is the commonly used enteral feeding technology. The clinical risks caused by tube dislodgement and peristomal site infection are the common complications before complete tract maturation after gastrostomy. However, there is currently no relevant research to promote gastrostomy wound treatment and tract maturation. Herein, a nanozyme loaded bioactive hydrogels (MO-HPA) was developed to accelerate tract maturation and inhibit bacteria. Nano-manganese dioxide (n-MO) and polylysine modified hyaluronic acid (HP) were synthesized and characterized. In situ hydrogels were prepared by mixing the HP/ alginate solution, and the n-MO solution containing Ca . The structure, physicochemical and mechanical properties of MO-HPA were evaluated. Furthermore, the antibacterial activity, and the In vitro and intracellular oxygen production efficacy were determined. The cell migration, wound healing and tube tract maturation promotion effect were assessed in cell experiments and in skin defect mouse model, as well as rabbit gastrostomy model. The n-MO has a uniform particle size with oxygen producing activities. The MO-HPA demonstrated a homogeneous and porous microstructure. Additionally, the gelation time, swelling ratio, rheological behavior, and mechanical properties of hydrogels could be tuned by adjusting the HP content. The antibacterial efficiency of the MO-HPA group on and increased by about 40.1% and 55.6% respectively, compared to the MO-HPA group. Additionally, MO-HPA hydrogel demonstrated effective oxygen-producing and cell migration-promoting functions in both in vitro and cellular experiments. The MO-HPA group significantly accelerated wound healing in both of mouse skin defect model and rabbit gastrostomy model. The hydrogel group exhibited a significant promotion in collagen content and reduction in HIF-1α, which effectively hastened tract maturation. Therefore, our study provides new and critical insights into a strategy to design bioactive hydrogels with multiple functions, which can open up a new avenue for accelerated wound healing after gastrostomy.

The development of biological macromolecule hydrogel dressings with fatigue resistance, sufficient mechanical strength, and versatility in clinical treatment is critical for accelerating full-thickness healing of skin wounds. Therefore, in this study, multifunctional, biological macromolecule hydrogels based on a recombinant type I collagen/chitosan scaffold incorporated with a metal–polyphenol structure were fabricated to accelerate wound healing. The resulting biological macromolecule hydrogel possesses sufficient mechanical strength, fatigue resistance, and healing properties, including antibacterial, antioxygenic, self-healing, vascularization, hemostatic, and adhesive abilities. Chitosan and recombinant type I collagen formed the scaffold network, which was the first covalent crosslinking network of the hydrogel. The second physical crosslinking network comprised the coordination of a metal–polyphenol structure, i.e., Cu2+ with the catechol group of dopamine methacrylamide (DMA) and stacking of DMA benzene rings. Double-crosslinked networks are interspersed and intertwined in the hydrogel to reduce the mechanical strength and increase its fatigue resistance, making it more suitable for clinical applications. Moreover, the biological macromolecule hydrogel can continuously release Cu2+, which provides strong antibacterial and vascularization properties. An in vivo full-thickness skin defect model confirmed that multifunctional, biological macromolecule hydrogels based on a recombinant type I collagen/chitosan scaffold incorporated with a metal–polyphenol structure can facilitate the formation of granulation tissue and collagen deposition for a short period to promote wound healing. This study highlights that this biological macromolecule hydrogel is a promising acute wound-healing dressing for biomedical applications.

As micron-sized objects, mobile microrobots have shown significant potential for future biomedical applications, such as targeted drug delivery and minimally invasive surgery. However, to make these microrobots viable for clinical applications, several crucial aspects should be implemented, including customizability, motion-controllability, imageability, biodegradability, and biocompatibility. Developing materials to meet these requirements is of utmost importance. Here, a gelatin methacryloyl (GelMA) and (2-(4-vinylphenyl)ethene-1,1,2-triyl)tribenzene (TPEMA)-based multifunctional hydrogel with 3D printability, fluorescence imageability, biodegradability, and biocompatibility is demonstrated. By using 3D direct laser writing method, the hydrogel exhibits its versatility in the customization and fabrication of 3D microstructures. Spherical hydrogel microrobots were fabricated and decorated with magnetic nanoparticles on their surface to render them magnetically responsive, and have demonstrated excellent movement performance and motion controllability. The hydrogel microstructures also represented excellent drug loading/release capacity and degradability by using collagenase, along with stable fluorescence properties. Moreover, cytotoxicity assays showed that the hydrogel was non-toxic, as well as able to support cell attachment and growth, indicating excellent biocompatibility of the hydrogel. The developed multifunctional hydrogel exhibits great potential for biomedical microrobots that are integrated with customizability, 3D printability, motion controllability, drug delivery capacity, fluorescence imageability, degradability, and biocompatibility, thus being able to realize the real in vivo biomedical applications of microrobots.