Living cells use chemical building blocks (biopolymers) to form fascinatingly complex architectures, which in turn display multiple functions necessary for the cell life cycle. The mechanisms and order of events by which forerunners of these extant biopolymers formed on the early earth remains under intensive investigation. Prebiotic chemistry research has recently provided ample evidence that both peptide and nucleic‐acid (NA) precursors could be formed in a primordial environment through common synthetic routes. However, until recently, studies directed at the design of functional supramolecular structures have focused primarily on assemblies made of either peptides or NAs. The emerging discipline of Systems Chemistry now develops dynamic supramolecular interactions to capture the complex emergent properties of reaction networks. Accordingly, we review here recent work that reveals mutualistic nucleic acid/peptide co‐assembly, and approaches toward utility of these architectures as functional materials capable of substrate binding, catalysis, replication, and translation. Many of these new approaches to smart soft biomaterials and functional bio‐nanotechnology provide insight and extend our understanding of the possible origins of living systems.

Recent attempts to develop the next generation of functional biomaterials focus on systems chemistry approaches exploiting dynamic networks of hybrid molecules. This task is often found challenging, but we herein...