Jianfu Zhang

Self-regulating soft actuators that combine large, reprogrammable shape-morphing with mechanical robustness are essential for next-generation bioinspired sensors and soft robotics, yet water-triggered systems often suffer from weak hydrogel mechanics, delamination in multilayers, and limited autonomous regulation. Here, we report a pinecone-scale-inspired, integrated bilayer polyurethane actuator in which a hydrophobic polycaprolactone (PCL)-rich layer and a hydrophilic polyethylene glycol (PEG)/PCL layer are molecularly fused via dynamic oxime bonds to eliminate interfacial failure while enabling healability. Leveraging the intrinsic contrast in semi-crystallinity and hydrophilicity of the soft segments, we create a single-material platform with dual-force competition between swelling pressure and thermally activated shape memory recovery. At 20 °C, the actuator bends continuously from 0° to 360°, reaching a maximum bending angle of 360° at 1140 s, after which the bending angle remains stable, with the bending trajectory and final geometry precisely tuned by the PCL/PEG feed ratio and laminate angle. Under wet-heat conditions, it also shows reversible transparent–opaque transitions, enabling coupled actuation and visual hygrothermal reporting. This strategy offers a robust route to programmable hygrothermal actuators for underwater sensing, soft grippers, and bioelectronic interfaces.

Natural communication methods have influenced the creation of sophisticated artificial materials capable of coherent and abundant responses to stimuli, a crucial necessity for developing applications such as dynamic encryption systems and high‐density information storage. However, existing materials for encryption and information storage are limited by predictable, single‐stimulus responses and lack the capacity for dynamic, continuous, and programmable changes. To address this gap, a bioinspired multicolor fluorescent polyurethane actuator is developed that combines dynamic color and shape adaptability within a single material platform. This smart actuator mimics the turgor‐driven movements of Oxalis corniculata through a hydrophilic/hydrophobic network that enables water diffusion, hydrogen bonding, and dynamic bond exchange. It responds to multiple stimuli, including temperature, pH, and excitation wavelength, exhibiting reversible multi‐state deformations and programmable fluorescence across red, green, blue, and even white light. The deformation behavior is supported by finite element simulations, ensuring precise control and predictability. Additionally, the tunable trichromatic fluorescence of the actuator underpins a 3D and 4D information encoding system, demonstrating increased information storage capacity and encryption security. The employment of micro‐processing technology in the fabrication of micro‐hidden optical encryption chips has been demonstrated, thus paving the way for underwater communication encryption technologies and adaptive materials.