Wheat gluten (WG) is a promising base material for production of "green" plastics, although reinforcement is needed in more demanding applications. Hemp fiber is a promising reinforcement source but difficulties exist in obtaining desired properties with a WG-based matrix. This study aimed at improving fiber dispersion and fiber-matrix interactions using a high speed blender and a diamine as a cross-linker. Samples were manufactured using compression molding, two types of blenders and addition of diamine. Mechanical properties were assessed with tensile testing. Tensile-fractured surfaces were examined with scanning electron microscopy (SEM). Protein polymerization and fiber-protein matrix interactions were examined using high performance liquid chromatography (HPLC) and confocal laser scanning microscopy (CLSM). The results showed that a higher-speed grinding yielded a more even distribution of fibers and a more polymerized protein structure compared to a lower-speed grinding. However, these improvements did not result in increased strength, stiffness, and extensibility for the higher-speed grinding. The strength was increased when the grinding was combined with addition of a diamine (Jeffamine(R) EDR-176). HPLC, SEM, and CLSM, indicated that diamine added samples showed a more "plastic" appearance together with a stiffer and stronger structure with less cracking compared to samples without diamine. The use of the diamine also led to an increased polymerization of the proteins, although no effect on the fiber-protein matrix interactions was observed using microscopical techniques. Thus, for future successful use of hemp fibers to reinforce gluten materials, an appropriate method to increase the fiber-protein matrix interaction is needed.