The resistance that microorganisms exert against antimicrobial agents is increasingly causing alarming issues globally. The problems and limitations associated with majority of the antimicrobial medications that have been designed to tackle microbial pathogens have necessitated the search for efficient techniques that will solve these problems. These problems and limitations have been taken care of since the advent of nanotechnology as it offers encapsulation of bioactive molecules within the nanoparticles and then release same in a carefully controlled manner that will enable the active molecules to reach target sites in a timely and efficient mechanism. There are numerous ways of achieving this but plant-based nanomaterials are promising methods because of their abundant bioactive repository, biocompatibility and eco-friendliness. This chapter highlights the techniques of plant-based nanomaterials in the regulated release of antimicrobial biomolecules. It explores how nanomaterials and biomolecules interact, and how these systems might be practically used to treat microbial diseases. This approach is however not free of shortcomings and some other limitations. Nonetheless, compared with other strategies used in antimicrobial chemotherapy, it offers a creative and sustainable response to the world’s healthcare problems by utilizing the complementary properties of antimicrobial biomolecules and plant-derived nanotechnology. Controlled release of antimicrobial biomolecules using plant-based nanomaterials not only serves as alternative to disease treatment but also improves the outcomes of treatment.