| Summary: | For fiber technology, new approaches such as biomimetic materials, such as silks, are being intensively explored, providing new solutions for a variety of industries, including textiles, composites, and biomedical engineering. New approaches for spinning or these materials are needed. Despite recent advances in enhancing fiber tensile properties, achieving significant improvement in tensile properties remains a tedious and challenging task, suffering from little to no controlled extrusion process and difficult optimization in high‐dimensional parameter spaces. Herein, a novel robotic biomimetic pulling method that can rapidly enhance fiber tensile properties surpassing current methods in both speed and resulting fiber properties is shown. Using a controlled fiber‐pulling device with in situ tensile measurements and adaptive optimization based on Bayesian Optimization, fiber strength exceeding 300% of the traditional full factorial design method within just a few experimental iterations is reached. The rapid experimental method presents a potential avenue for enhancing the performance of artificial fibers across diverse industries and applications.
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