hROS‐Responsive Behavior for Long‐Term Stability of Cellulosic Gold Nanoclusters

Abstract Understanding the gold core‐ligand interaction in gold nanoclusters (GNCs) is essential for the on‐demand tailoring of their photoluminescence properties and long‐term stability. Here, inspired by the suckers arranged directionally on the tentacles of octopus, a series of GNCs with regulating ligand structures are grown and stabilized on the cellulose nanocrystals (CNCs). The carboxylated CNCs providing an electron‐rich environment to promote the luminescence of GNCs and stabilize it within a long‐term of 1 year through anchoring and diluting effects, and the highest quantum yields reaches 31.02% in ultrapure water. Interestingly, this bionic preparation strategy is generally applicable to various ligands for tailoring on‐demand hROS‐responsive and nonresponsive GNCs to construct tunable‐emission wavelength dual GNCs ratiometric probes. The results show that designing a specific ligand structure to inhibit the transformation of Au‐Au to Au (I)‐ligand in GNCs is crucial to regulate the hROS‐responsive characteristics. As expected, the interfacial compatible dual GNCs ratiometric probe with a hROS limit of detection of 0.74 µmol L⁻¹ can diagnose certain diseases through intracellular hROS imaging. This work provides important insights for understanding the gold core‐ligand interaction in GNCs during the oxidation process triggered by intracellular hROS.