The establishment of the bond of sessile marine organisms such as barnacles, mussels, and algae in the marine environment starts with the secretion and the adsorption of the adhesive biopolymers to the substrate. Subsequently, this is followed by the formation of cohesive interactions with the next layer of adhesive biopolymers that are deposited ladsorbed on top of the first layer. These two fundamental processes for the adhesive plaque buildup have been subjected to several investigations in recent years using model molecules, especially Mefp-1 extracted from the blue mussel Mytilus edulis. With the introduction of optical surface-sensitive methods such as ellipsometry, surface plasmon resonance (SPR), and infrared spectroscopy (IR), it has been possible to elucidate both the kinetics of adsorption and structure of the Mefp-1 film. In contrast to adsorption, the cohesive interactions or the cross-linking are not easily followed with these optical methods and new approaches and techniques are required. One such technique that has been useful is the quartz-crystal microbalance with dissipation monitoring (QCM-D), which has been used for cross-linking studies of a variety of biopolymers including bioadhesives from mussel and algae.