PEG‐Induced Controllable Thin−Thickness Gradient and Water Retention: A Simple Way to Programme Deformation of Hydrogel Actuators

Abstract Building the differential growth through the thickness is a promising and challenging approach to design the morphing structures of hydrogel actuators. Besides retaining the size of the hydrogel actuators under environmental stimuli still remains a big challenge. Herein, a facile and universal approach is developed to address both issues by introducing PEG during the polymerization of N‐isopropylacrylamide (NIPAm) via one step method using asymmetric mold. Both composition gradient and pore gradient are obtained in micro level along the thickness direction of the final hydrogel, while thin‐thickness gradient in macro level. The thickness gradient and water retention can be controllably adjusted by changing PEG concentration. The introduction of PEG effectively improves both responsive and non‐shrunken performance by the interaction with PNIPAm. The resultant anisotropic PNIPAm/PEG hydrogel respond quickly and reach maximum deformation (360°) within 10 s at low temperature (40 °C). The various 3D shape and biomimetic movement can be programmed by simply controlling the PEG concentration and mold shape. This strategy can provide new insights into the design intelligent soft materials with 3D morphing for bioinspired and biomedical applications.