The development of mussel-inspired materials with enhanced mechanical and physiological characteristics is fascinating due to the resulting structural properties. In this work, based on a chemical reaction, 3-(3,4-dihydroxyphenyl)propionic acid and dopamine hydrochloride (DA), with a catechol group, were covalently grafted onto a bio-compatible polymer backbone of chitosan hydrochloride (CHI) and hyaluronic acid sodium (HA). A mussel-inspired water-resistant adhesive film that could adhere in water was then fabricated by an environmentally friendly layer-by-layer (LbL) process. The water-resistant adhesive film demonstrated a strong underwater mechanical connection (0.82 ± 0.19 MPa) and a high transmittance (more than 83%) in the visible region; these characteristics are beneficial for clinical observation. A free-standing water-resistant adhesive film with a high transmittance of over 83% was also demonstrated and obtained from a facial and effective mechanical exfoliation method. The free-standing film exhibited favorable adhesion capacity with porcine skin, making it attractive for applications in the biomedical field.
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