In this study, mussel-inspired chemistry, based on catechol-amine reactions, was adopted to develop self-cross-linkable chitosan-alginate (Chi-Alg) complexes. To do so, the biopolymers were each substituted with ∼20% catechol groups (ChiC and AlgC), and then four complex combinations (Chi-Alg, ChiC-Alg, Chi-AlgC, ChiC-AlgC) were prepared at the surface and in bulk solution. Based on QCM-D and lap shear adhesion tests, the complex with catechol only on Chi (ChiC-Alg) did not show a significant variation from the control complex (Chi-Alg). Conversely, the complexes with catechol on alginate (Chi-AlgC and ChiC-AlgC) rendered a self-cross-linking property and enhanced cohesive properties.