Achieving multifunctional shape changing hydrogels with synergistic and engineered material properties is highly desirable for their expanding applications, yet remains an ongoing challenge. The synergistic design of multiple dynamic chemistries enables new directions for development of such materials. Herein, we propose a molecular design strategy based on hydrogel combining acid-ether hydrogen bonding and imine bonds. Our approach utilizes simple and scalable chemistries to produce a doubly dynamic hydrogel network, which features high water uptake, high strength and toughness, excellent fatigue-resistance, fast and efficient self-healing, as well as superfast, programmable shape changing. Furthermore, deformed shapes could be memorized due to a large thermal hysteresis. This new type of shape changing hydrogel is expected to be a key component in future biomedical, tissue and soft robotic device applications.

Dynamic bonds have achieved significant attention for their ability to impart fascinating properties to polymeric materials, such as high mechanical strength, self‐healing, shape memory, 3D printability, and conductivity. Incorporating multiple dynamic bonds into polymer systems affords an attractive and efficient approach to endow multiple functionalities. This mini‐review focuses on the use of complementary dynamic interactions to control the properties of soft materials. Owing to the diversity in dynamic chemistries that can be explored, the scope of this article is restricted to polymers and does not include colloids, amphiphiles, liquid crystals, or biological soft matter.