Spider silk is the toughest fiber in the natural world. By introducing β-sheet crystals and α-helical peptides simultaneously in a pseudoprotein polymer, as described in article number 1904311, Jinlian Hu and co-workers prepare a supertough artificial spider silk using a facile chemical synthesis route. The toughness (≈387 MJ m−3) is more than twice the reported value of common spider dragline silk.