Natural Polymer‐Polyphenol Bioadhesive Coacervate with Stable Wet Adhesion, Antibacterial Activity, and On‐Demand Detachment

Medical adhesives are emerging as an important clinical tool as adjuvants for sutures and staples in wound closure and healing and in the achievement of hemostasis. However, clinical adhesives combining cytocompatibility, as well as strong and stable adhesion in physiological conditions, are still in demand. Herein, a mussel‐inspired strategy is explored to produce adhesive coacervates using tannic acid (TA) and methacrylate pullulan (PUL‐MA). TA|PUL‐MA coacervates mainly comprise van der Waals forces and hydrophobic interactions. The methacrylic groups in the PUL backbone increase the number of interactions in the adhesives matrix, resulting in enhanced cohesion and adhesion strength (72.7 Jm−2), compared to the non‐methacrylated coacervate. The adhesive properties are kept in physiologic‐mimetic solutions (72.8 Jm−2) for 72 h. The photopolymerization of TA|PUL‐MA enables the on‐demand detachment of the adhesive. The poor cytocompatibility associated with the use of phenolic groups is here circumvented by mixing reactive oxygen species‐degrading enzyme in the adhesive coacervate. This addition does not hamper the adhesive character of the materials, nor their anti‐microbial or hemostatic properties. This affordable and straightforward methodology, together with the tailorable adhesivity even in wet environments, high cytocompatibility, and anti‐bacterial activity, enables foresee TA|PUL‐MA as a promising ready‐to‐use bioadhesive for biomedical applications. An adhesive coacervate formed by tannic acid and methacrylate pullulan through supramolecular interactions, with stable wet adhesion, high cytocompatibility, antibacterial activity, and hemostatic properties, is reported. The use of photopolymerizable groups leads to the development of an on‐demand detachment adhesive. The new biomaterial is designed for wound closure and healing, being a promising bioadhesive for biomedical applications.