Polyurethane (PU) has been widely used as a glue in various areas. However, adhesion in the presence of water is greatly impeded and results in most synthetic adhesive failure. In this study, we designed and synthesized a novel PU construction; underwater PU adhesives were created by the incorporation of synthetic glycerol monomethacrylate (GMA). Furthermore, the urethane structure helped the adhesive eliminate the interfacial water barrier through interactions that were stronger than hydrogen bonding, and GMA as a crosslinking agent was used to generate post-covalent-crosslinking networks through radical polymerization. This enhanced the cohesion so the diffusion of water molecules could be overcome. Fourier transform infrared spectroscopy, thermogravimetric analysis, underwater adhesion measurements, and tensile tests were used to characterize the chemical and mechanical properties of the as-obtained adhesive. This led to an adhesive with a better mechanical strength and interfacial adhesion in water, and the results show that the mechanical properties (tensile strength, Young's modulus, and tensile elongation) of the GMA-PU adhesive were higher than those of the pure PU. As for the 4% GMA, the tensile strength was enhanced by 24.3% and the elongation was enhanced by 125.23% over those of the pure PU. This confirmed that the incorporation of GMA into the PU matrix indeed induced increasing cohesion, and the sample's adhesive strength was 21.19 6 3.9 MPa; this indicated a superior adhesive strength over that of the pure PU. In addition, we can foresee that underwater adhesion will play an important role in prospective surgery and engineering areas. V C 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018, 135, 46579.