Natural spider silks with striking performances achieve extensive investigations. Nonetheless, a lack of consensus over the mechanism of the natural spinning hinders the development of artificial spinning methods where the regenerated spider silks generally show poor performances compared with the natural fibers. As is known, the Plateau–Rayleigh instability tends to break solution column into droplets and is considered a main challenge during fiber‐spinning. Here in this study, by harnessing the viscoelastic properties of the regenerated spidroin dope solution via organic salt–zinc acetate (ZA), this outcome can be avoided, and dry‐spinning of long and mechanically robust regenerated spider silk ribbons can be successfully realized. The as‐obtained dry‐spun spider silk ribbons show an enhanced modulus up to 14 ± 4 GPa and a toughness of ≈51 ± 9 MJ m−3 after the post‐stretching treatment, which is even better than that of the pristine spider silk fibers. This facile and flexible strategy enriches the spinning methodologies which bypass the bottleneck of precisely mimicking the complex natural environment of the glands in spiders, shining a light to the spider‐silk‐based textile industrial applications.
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