An investigation was undertaken on the application of dilute chitosan solutions gelled by melB tyrosinase-catalyzed reaction with 3,4-dihydroxyphenethylamine (dopamine). The tyrosinase-catalyzed reaction with dopamine conferred water-resistant adhesive properties to the semi-dilute chitosan solutions. The viscosity of the chitosan solutions highly increased by the tyrosinase-catalyzed quinone conversion and the subsequent nonenzymatic reactions of o-quinones with amino groups of the chitosan chains. The viscosity of chitosan solutions highly increased in shorter reaction times by addition of melB tyrosinase. Therefore, in this study, the gelation of a chitosan solution was carried out without poly(ethylene glycol) (PEG), which was added for the gelation of chitosan solutions using mushroom tyrosinase. The highly viscous, gel-like modified chitosan materials were allowed to spread onto the surfaces of the glass slides, which were tightly lapped together and were held under water. Tensile shear adhesive strength of over 400 kPa was observed for the modified chitosan samples. An increase in either amino group concentration of the chitosan solutions or molecular mass of the chitosan samples used effectively led to an increase in adhesive strength of the glass slides. Adhesive strength obtained by chitosan materials gelled enzymatically was higher than that obtained by a chitosan gel prepared with glutaraldehyde as a chemical crosslinking agent. In addition, the use of melB tyrosinase led to a sharp increase in adhesive strength in shorter reaction times without other additives such as PEG.