Citation: Yi Zhang, Xin Yao, Jiaxin Yu, Haili Qin, Huaiping Cong. Gradient crosslinking of anisotropic hydrogels for programmable shape morphing and actuation[J]. Chinese Chemical Letters, ;2026, 37(6): 112041. doi: 10.1016/j.cclet.2025.112041 shu

Gradient crosslinking of anisotropic hydrogels for programmable shape morphing and actuation

Anhui Province Engineering Research Center of Flexible and Intelligent Materials, School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei 230009, China

xyao@mail.hfut.edu.cn

hpcong@hfut.edu.cn

Received Date: 26 July 2025
Revised Date: 23 October 2025
Accepted Date: 30 October 2025
Available Online: 31 October 2025

Figures(5)

Biological systems exploit their sophisticated hierarchical anisotropic architectures to achieve complex shape morphing under external stimuli. However, artificial soft intelligent actuators often suffer from limited response speeds and poor programmability of deformation, primarily due to densely crosslinked network designs and insufficient anisotropic resolution. Here, we report a synergistic method combining directional freezing-induced self-assembly and dynamic metal coordination crosslinked mechanical alignment to fabricate anisotropic hydrogels with fast multiple responsiveness and programmable three-dimensional (3D) deformation. Benefiting from an interconnected lamellar network and open-oriented mass transport channels, the hydrogel exhibits rapid anisotropic stimuli-responsive deformations with a shrinkage along the lamellar direction that is 1.9 times greater than that in the perpendicular direction in 5 s of thermal stimulation, and a complete recovery within 4 s upon cooling. By developing a spatially modulated coordination photodissociation strategy, a gradient crosslinking network is further constructed within the hydrogel, enabling diverse and programmable 3D deformations in response to external stimuli, which facilitate complex actuation behaviors such as object grasping, biomimetic gestures, and light-driven lifting. Thus, the hydrogel with hierarchically anisotropic structure and porous dynamic crosslinked network is potential for intelligent soft robotics requiring flexible controllable deformation.
- Anisotropic hydrogel,
- Gradient crosslinking,
- Lamellar alignment,
- Programmable shape morphing,
- Actuating performance
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