Spider silk is a fascinating material, combining high strength and elasticity that outperforms most synthetic fibers. Another intriguing feature of spider silk is its ability to “supercontract,” shrinking up to 50% when exposed to water. This is likely on account of the entropy‐driven recoiling of secondary structured proteins when water penetrates the spider silk. In contrast, humidity‐driven contraction in synthetic fibers is difficult to achieve. Here, inspired by the spider silk model, a supercontractile fiber (SCF), which contracts up to 50% of its original length at high humidity, comparable to spider silk, is reported. The fiber exhibits up to 300% uptake of water by volume, confirmed via environmental scanning electron microscopy. Interestingly, the SCF exhibits tunable mechanical properties by varying humidity, which is reflected by the prolonged failure strain and the reversible damping capacity. This smart supramolecular fiber material provides a new opportunity of fabricating biomimetic muscle for diverse applications.

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