Exploring Stimuli-Responsive Natural Processes for the Fabrication of High-Performance Materials.

Climate change and environmental pollution have underscored the urgency for more sustainable alternatives in synthetic polymer production. Nature's repertoire of biopolymers with excellent multifaceted properties alongside biodegradability could inspire next-generation innovative green polymer fabrication routes. Stimuli-induced processing, driven by changes in environmental factors, such as pH, ionic strength, and mechanical forces, plays a crucial role in natural polymeric self-assembly process. This perspective aims to close the gap in understanding biopolymer formation by highlighting the essential role of stimuli triggers in facilitating the bottom-up fabrication, allowing for the formation of intricate hierarchical structures. In particular, this perspective will delve into the stimuli-responsive processing of high-performance biopolymers produced by mussels, caddisflies, velvet worms, sharks, whelks, and squids, which are known for their robust mechanical properties, durability, and wet adhesion capabilities. Finally, we provide an overview of current advancements and challenges in understanding stimuli-induced natural formation pathways and their translation to biomimetic materials.