With improved understanding of the design rules for self-assembling peptides, new challenges will be faced to incorporate these materials into dynamic systems of higher complexity and functionality. In this highlight article we discuss very recent advances in these areas. Three areas are covered: (i) molecular networks based on peptides and their interactions including (bio-) catalytically driven systems; (ii) supramolecular functionality, both in the context of biological and nanotechnology applications; (iii) approaches to effectively interface peptides with synthetic and biological materials. We also discuss challenges and opportunities for the design of a new generation of peptide nanomaterials for the next decade.