Silk producing arthropods spin solid fibres from an aqueous protein feedstock apparently relying on the complex structure of the silk protein and its controlled aggregation by shear forces, alongside biochemical changes. This flow-induced phase-transition of the stored native silk molecules is irreversible, environmentally sound and remarkably energy efficient. The process seemingly relies on a self-assembling, fibrillation process. Here we test this hypothesis by biomimetically spinning a native-based silk feedstock, extracted by custom processes, into silk fibres that equal their natural models’ mechanical properties. Importantly, these filaments, which featured cross-section morphologies ranged from large crescent-like to small ribbon-like shapes, also had the slender cross-sectional areas of native fibres and their hierarchical nanofibrillar structures. The modulation of the post-draw conditions directly affected mechanical properties, correlated with the extent of fibre crystallinity, i.e. degree of molecular order. We believe our study contributes significantly to the understanding and development of artificial silks by demonstrating successful biomimetic spinning relies on appropriately designed feedstock properties. In addition, our study provides inspiration for low-energy routes to novel synthetic polymers.
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