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As a natural "binder," lignin fixes cellulose in plants to foster growth and longevity. However, isolated lignin has a poor binding ability, which limits its biomedical applications. In this study, inspired by mussel adhesive proteins, acidic/basic amino acids (AAs) are introduced in alkali lignin (AL) to form ionic-π/spatial correlation interactions, followed by demethylation to create catechol residues for enhanced adhesion activity. Atomic force microscopy reveals that catechol residues are the primary adhesion structures, with basic AAs exhibiting superior synergistic effects compared to acidic AAs. Demethylated lysine-grafted AL exhibits the strongest adhesion force toward skin tissue. Molecular dynamic simulation and density functional theory calculations indicate that adhesion against skin tissue mainly results from hydrogen bonds and cation-π interactions, with the adhesion mechanism being based on the Gibbs free energy of the Schiff base reaction. In summary, a biomimetic electrode based on lignin inspired by mussel adhesive proteins is prepared; the presented method offers a straightforward strategy for the development of biomimetic adhesives. Furthermore, this mussel-inspired adhesive can be used as a wearable bioelectrode in biomedical applications., (© 2024 Wiley‐VCH GmbH.)