Polysaccharide multilayers consisting of hyaluronic acid and chitosan were prepared by layer-by-layer assembly. To be used in seawater, the multilayers were crosslinked to a different degree using thermal or chemical methods. ATR-FTIR revealed different amide densities as a result of the crosslinking conditions. AFM showed that the crosslinking affected the roughness and swelling behavior of the coatings. The stability and degradability of the multilayers in aqueous environments were monitored with spectroscopic ellipsometry. The resistance of the coatings against non-specific protein adsorption was characterized by SPR spectroscopy. Settlement assays using zoospores and removal assays using the diatom showed that the slowly degradable coatings were less prone to fouling than the strongly crosslinked ones. Thus, the coatings were a suitable model system to show that crosslinking the multilayers under mild conditions and equipping the coatings with controlled degradation rates enhances their antifouling and fouling-release properties against marine fouling organisms.