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Abstract Synthetic macrocycles have served as principal tools for supramolecular chemistry since their establishment, and the investigation of macrocycles‐aided organic‐inorganic hybrid nanomaterials has also attracted broad interest in chemistry and material communities during the past decade owing to their widespread applications in optical sensing, catalytic degradation, biomedicine, and other related fields. Herein, a new class of silver nanoparticles (AgNPs) modified by anionic water‐soluble [2]biphenyl‐extended pillar[6]arene (WBpP6), namely WBpP6‐AgNPs, is designed and synthesized through a facile one‐pot method. WBpP6‐AgNPs with good dispersion and stability exhibit efficient catalytic properties toward the hydrogenation of a series of aromatic nitro compounds and also show good performance in label‐free detection toward diquat.