This chapter describes peptide design strategies for the construction of nanostructured materials. It begins with a brief tutorial of amino acid structure and function and then describes higher-order assemblies of peptides and peptidomimetics. Primarily β-sheet fibril-forming peptides and α-helical coiled coil systems are discussed, as these systems have received particular attention in recent years for building nanostructured materials. Useful properties that arise from peptide construction are addressed, including stimulus-responsiveness, modularity, and multifunctionality, and a number of technological applications are described, including Tissue Engineering, antimicrobials, drug delivery, and nanoscale electronics. The chapter is meant to be an introduction for researchers or students in nanotechnology who may wish to extend their approaches into the biomolecular realm, and it also provides a compendium of recent advances for experts in the field of nanoscale peptide materials.