Antimicrobial-resistant (AMR) bacteria are unequivocally identified as the most important global threat to human, animal and plant health in the 21st century. In humans, AMR is predicted to outstrip cancer, cardiovascular, neurological and metabolic disorders as the most important cause of death by 2050. Tackling AMR requires multidisciplinary approaches, including the repurposing and revitalization of older drugs, development of new compounds and novel strategies to deliver them for treating and preventing the spread of multidrug-resistant bacterial infections. In this chapter, research exploiting supramolecular peptide nanotechnology for the development of antimicrobial nanomaterials is summarized, with particular emphasis on the role of molecular design and self-assembly in harnessing antimicrobial activities