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Nature builds biological materials from limited ingredients, however, with unparalleled mechanical performances compared to artificial materials, by harnessing inherent structures across multi‐length‐scales. In contrast, synthetic material design overwhelmingly focuses on developing new compounds, and fails to reproduce the mechanical properties of natural counterparts, such as fatigue resistance. Here, a simple yet general strategy to engineer conventional hydrogels with a more than 100‐fold increase in fatigue thresholds is reported. This strategy is proven to be universally applicable to various species of hydrogel materials, including polysaccharides (i.e., alginate, cellulose), proteins (i.e., gelatin), synthetic polymers (i.e., poly(vinyl alcohol)s), as well as corresponding polymer composites. These fatigue‐resistant hydrogels exhibit a record‐high fatigue threshold over most synthetic soft materials, making them low‐cost, high‐performance, and durable alternatives to soft materials used in those circumstances including robotics, artificial muscles, etc.
Fatigue‐resistant hydrogels are fabricated through synergistically engineering the preferentially aligned microstructures and nanocrystalline domains, enabling application as load‐bearing components in underwater robots.