Flexoelectric Polarization‐Enhanced Gd‐Based Nanoflowers for Efficient Phosphatase‐Mimicking Dephosphorylation

Phosphatase‐mimicking nanozymes provide highly stable enzyme‐like activity but remain limited by their static catalytic nature. Herein, this study achieves flexoelectricity‐driven dynamic modulation of nanozyme activity by employing gadolinium‐based nanoflowers (GNF) with hierarchical ultrathin architectures. These structures possess curvature‐induced strain gradients and hydroxyl‐rich surfaces, which generate pronounced flexoelectric polarization under mild ultrasonic excitation. Finite element simulations reveal that mechanical loading induces localized strain gradients and surface potential anisotropy, forming a structural basis for dynamic interfacial charge redistribution. Density functional theory calculations demonstrate that flexoelectric polarization lowers the activation barrier and shifted the rate‐determining step, transforming the reaction pathway. This polarization enhances the Lewis acidity of Gd 3+ sites and stabilized transition states, thereby accelerating phosphate ester hydrolysis. The GNF nanozyme exhibits excellent phosphatase‐like catalytic activity and enables the ultrasensitive colorimetric detection of biologically relevant targets, such as bovine serum albumin and fluoride ions, with low detection limits and robust matrix tolerance. This study pioneers the integration of strain‐gradient‐induced polarization into nanozyme catalysis, establishing a generalizable framework for constructing adaptive and mechanically responsive artificial enzymes.