Bridging stimulus-responsive and dissipative peptide assemblies to build complex interactive biomaterials.

Self-assembling peptides are versatile building blocks for biomaterials owing to their programmable sequences and ability to form complex supramolecular architectures. Designing systems that operate dynamically at the biological interface is particularly compelling, as living systems rely on both stimulus responsiveness and continuous energy dissipation to regulate structure and function. However, most synthetic peptide assemblies remain confined to near-equilibrium behaviour, whereas chemically fuelled dissipative systems often lack compatibility with biological environments. In this Review, we discuss recent advances in stimulus-responsive and dissipative peptide assemblies, highlighting their distinct design principles and functional capabilities. We compare sequence-encoded and trigger-based strategies with chemically fuelled reaction networks that enable transient assembly. Finally, we outline emerging strategies to bridge these approaches, including improving bioorthogonality, tuning concentration regimes, and integrating cellular processes. Together, these concepts provide a framework for developing interactive peptide biomaterials with life-like functions.