Due to the abuse of antibiotics and the emergence of multidrug resistant microorganisms, medical devices, and related biomaterials are at high risk of microbial infection during use, placing a heavy burden on patients and healthcare systems. Metal–phenolic networks (MPNs), an emerging organic–inorganic hybrid network system developed gradually in recent years, have exhibited excellent multifunctional properties such as anti‐inflammatory, antioxidant, and antibacterial properties by making use of the coordination between phenolic ligands and metal ions. Further, MPNs have received widespread attention in antimicrobial infections due to their facile synthesis process, excellent biocompatibility, and excellent antimicrobial properties brought about by polyphenols and metal ions. In this review, different categories of biomaterials based on MPNs (nanoparticles, coatings, capsules, hydrogels) and their fabrication strategies are summarized, and recent research advances in their antimicrobial applications in biomedical fields (e.g., skin repair, bone regeneration, medical devices, etc.) are highlighted.

Chronic wounds, such as pressure ulcers, vascular ulcers and diabetic foot ulcers (DFUs), often stay in a state of pathological inflammation and suffer from persistent infection, excess inflammation, and hypoxia, thus they are difficult to be healed. Nitric oxide (NO) plays a critical role in the regulation of various wound healing processes, including inflammatory response, cell proliferation, collagen formation, antimicrobial action and angiogenesis. The important role of NO in wound healing attracts intensive research focus on NO-based wound healing therapy. However, the application of NO gas therapy needs to resolve the intrinsic shortcomings of gas therapy, such as short storage and release times as well as temporal and spatial uncontrollability of the release mode. So far, various types of NO donors, including organic nitrates (RONO₂), nitrites (RONO), S-nitrosothiols (RSNOs), nitrosamines, N-diazeniumdiolates (NONOates), and metal–NO complexes, have been developed to solidify gaseous NO and they were further encapsulated in or conjugated onto a variety of biomaterial vectors to develop NO delivery systems. NO synthetic enzyme mimics to catalyze the production and release of NO from L-arginine have also been developed. This paper reviews recent advances of NO donors, biomaterial vectors, thus-formed NO delivery systems, as well as recently emerged NO synthetic enzyme mimics. Furthermore, this review also summarizes the functions of NO releasing biomaterials that would benefit chronic wound healing, including antibacterial properties and the promotion of angiogenesis, as well as the convenient combination of light/thermal induced NO release with light/thermal therapies, and the prospects for future developing trends in this area.

The revolutionary role of tissue adhesives in wound closure, tissue sealing, and bleeding control necessitates the development of multifunctional materials capable of effective and scarless healing. In contrast to the use of traditionally utilized toxic oxidative crosslinking initiators (exemplified by sodium periodate and silver nitrate), herein, the natural polyphenolic compound tannic acid (TA) was used to achieve near instantaneous (<25s), hydrogen bond mediated gelation of citrate-based mussel-inspired bioadhesives combining anti-oxidant, anti-inflammatory, and antimicrobial activities (3A-TCMBAs). The resulting materials were self-healing and possessed low swelling ratios (<60%) as well as considerable mechanical strength (up to ∼1.0 MPa), elasticity (elongation ∼2700%), and adhesion (up to 40 kPa). The 3A-TCMBAs showed strong in vitro and in vivo anti-oxidant ability, favorable cytocompatibility and cell migration, as well as photothermal antimicrobial activity against both Staphylococcus aureus and Escherichia coli (>90% bacterial death upon near-infrared (NIR) irradiation). In vivo evaluation in both an infected full-thickness skin wound model and a rat skin incision model demonstrated that 3A-TCMBAs + NIR treatment could promote wound closure and collagen deposition and improve the collagen I/III ratio on wound sites while simultaneously inhibiting the expression of pro-inflammatory cytokines. Further, phased angiogenesis was observed via promotion in the early wound closure phases followed by inhibition and triggering of degradation & remodeling of the extracellular matrix (ECM) in the late stage (supported by phased CD31 (platelet endothelial cell adhesion molecule-1) PDGF (platelet-derived growth factor) and VEGF (vascular endothelial growth factor) expression as well as elevated matrix metalloprotein-9 (MMP-9) expression on day 21), resulting in scarless wound healing. The significant convergence of material and bioactive properties elucidated above warrant further exploration of 3A-TCMBAs as a significant, new class of bioadhesive.