Adhesive materials have been attracted for hemostatic agents, wound closure, and other applications towards medical devices and drug delivery platform due to their long-lasting properties in vivo. Polyphenol modification inspired by mussels’ adhesion and plant astringency has been emerging as a strategy to engineer robust, wet-resistant adhesive polymeric materials. Here, we present a variety of polyphenol adhesives for cardiovascular therapy, advanced 3D printing as well as tissue interfacing. Firstly, catechol modification onto chitosan permits unique polymeric phase transition from solid film to adhesive hydrogels, which is applicable to design ‘bloodless needles’ even after injection. Secondly, tannic acid widely found in plants is spontaneously complexed with proteins or choleteryl liquid crystals for cardiovascular applications. Lastly, such polyphenol-modified hydrogels can be useful as ink materials for advanced on-tissue 3D printing techniques. Ultimately, these nature-inspired adhesive materials would be useful for developing next generation of medical formulations for drug delivery and tissue repair.