Nature provides prime examples of lightweight, strong, stiff and tough materials. Their unique properties are realized via the hierarchical self-organizing growth of hard (inorganic, protein crystals, crystalline polysaccharides) and soft (organic, biopolymeric) building blocks into well-ordered structures with tailored energy dissipation mechanisms. Nacre, wood or silk are paradigms in materials design and considered near perfect marriages of hard and soft components. Additionally, other aspects of natural structural materials include their capability to adapt their mechanical properties on demand, or to combine mechanical properties with optical functions.

Herein, I will discuss large-scale self-assembly approaches to mimic the structures found in natural high performance materials, and focus on how to tune the mechanical and functional properties. This includes engineering and tailoring of sacrificial bonds, as well as Vitrimer approaches that allow for a complete recycling of bioinspired nanocomposites. Towards adaptive materials, I will discuss how to endow such materials with reconfigurable mechanical patterns using light, or achieve simple switching with electricity. Building on the organization principles of such bioinspired nanocomposites, I will also showcase approaches for functional materials design, including transient information storage using phosphorescent materials and lasers built from cellulose nanocrystals.