ABSTRACT Soft hydrogels capable of simultaneous shape morphing and optical modulation under a single stimulus hold promise for next‐generation intelligent materials. However, most systems rely on complex architectures or multi‐component triggers, limiting integration and responsiveness. Here, we develop a structurally homogeneous nanocluster–gel platform by embedding water‐soluble gold nanoclusters (AuNCs) into a polyacrylamide matrix, enabling synchronized mechanical deformation and tunable luminescence in response to solvent polarity. Upon exposure to organic solvents, the gel rapidly contracts (97% reversibility over 10 cycles. The integrated responsiveness is demonstrated in a biomimetic lotus‐shaped gel that folds and dims upon water uptake, and is further validated in a leakage scenario where the hydrogel serves as a pipe encapsulation film, achieving rapid sealing and visual monitoring of solvent leakage. This work establishes a nanocluster–gel platform that unifies photophysics and actuation for adaptive, self‐indicating soft systems.
Lin et al. (Thu,) studied this question.