A vinyl isocyanate (VI) synthesized from toluene diisocyanate and 2-hydroxyethyl methacrylate was used as a novel coupling agent to obtain strong chemical interfacial adhesion and therefore, improve the tensile properties of Kraft fiber-reinforced unsaturated polyester (UPE) composites. Results characterized by fourier transform infrared spectroscopy (FTIR), dynamic mechanical analysis (DMA), and scanning electron microscope (SEM) indicated that the novel coupling agent VI had a significant effect on the tensile properties of composites due to the formation of chemical bonds between the VI-Kraft interfaces and the VI-UPE interfaces. The tensile properties of composites modified by VI were much better than those of the control composite without VI modification. The VI-modified composites after severe hygrothermal aging exhibited lower losses of tensile properties and desirable tensile durability. The improvement in tensile properties, less interfacial separation after severe hygrothermal aging, lower damping values, and higher glass transition temperature are sufficient to show that the interfacial adhesion between the Kraft fiber and the UPE matrix was significantly improved because the coupling agent VI has both active isocyano groups which react with the Kraft fiber and vinyl groups which are copolymerizable with the UPE resin. (C) 2012 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 128:1036-1043, 2013