How to prepare a hydrogel with high strength and excellent tearing fracture energy is a problem faced by researchers. Here, tough and tear‐resistant double‐network hydrogels (Cx‐SMy gels) are successfully prepared via a facile strategy: micellar polymerization followed by solution polymerization. The strength and fracture energy of these hydrogels are up to 13 MPa and 26500 J m−2, respectively, which are attributed to the synergy of quatra‐crosslinking interactions inside the double‐network. The quatra‐crosslinking interactions include hydrophobic interaction, crystallization, electrostatic attraction, and hydrogen bonding. Moreover, it is confirmed that the facile strategy is a general way to prepare tough hydrogels by using electrolytic monomers and hydrophobic acrylates.
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