Natural fiber-reinforced biocomposites are increasingly used in various industries such as automotive, construction, biomedical, and recreation, thanks to their distinctive advantages over traditional glass fiber-reinforced plastics. Natural fiber composites are sustainable, environmentally friendly, low cost, low density, and easy to proc es sasw ella sha v ehi ghmec ha n ic alproperties. The quality of fiber-matrix interface is of critical importance since it determines the load distribution capability of the material. The interface between natural fibers and polymer resins has always been problematic because of the low compatibility between cellulose-based hydrophilic natural fibers and hydrophobic polymer resins, which leads to poor fiber-matrix adhesion and therefore inefficient load distribution between fibers and matrix. To date, several interfacial modification methods have been implemented to address this issue and improve the properties of the resulting composites. This chapter focuses on the interfacial modification of hemp fiber-based composites. First, hemp fiber structure and the nature of fiber-matrix interface were explained. Mechanisms of fiber/matrix adhesion as well as qualitative and quantitative methods for the determination of interface strength were outlined. Finally, the interface modification methods for hemp fiber-reinforced biocomposites were presented in the light of scientific literature.