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For double network (DN) hydrogels, their performance can be tuned by adjusting the interaction between their two networks. A novel DN hydrogel toughening approach is proposed by employing Janus nanoparticles (JNs) as crosslinkers to gain a conjoined‐network hydrogel. First, a kind of JNs modified by amino groups and quaternary ammonium salt is synthesized, named R3N+‐JN‐NH2. The DN hydrogel is fabricated...