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Abstract The spatial and temporal control of material properties at a distance has yielded many unique innovations including photo-patterning, 3D-printing, and architected material design. To date, most of these innovations have relied on light, heat, sound, or electric current as stimuli for controlling the material properties. Here, we demonstrate that an electric field can induce chemical reactions and subsequent polymerization in composites via piezoelectrically-mediated transduction. The response to an electric field rather than through direct contact with an electrode is mediated by a nanoparticle transducer, i.e., piezoelectric ZnO, which mediates reactions between thiol and alkene monomers, resulting in tunable moduli as a function of voltage, time, and the frequency of the applied AC power. The reactivity of the mixture and the modulus of a naïve material containing these elements can be programmed based on the distribution of the electric field strength. This programmability results in multi-stiffness gels. Additionally, the system can be adjusted for the formation of an electro-adhesive. This simple and generalizable design opens avenues for facile application in adaptive damping and variable-rigidity materials, adhesive, soft robotics, and potentially tissue engineering. 

Abstract Programmable mechanically active materials (MAMs) are defined as materials that can sense and transduce external stimuli into mechanical outputs or conversely that can detect mechanical stimuli and respond through an optical change or other change in the appearance of the material. Programmable MAMs are a subset of responsive materials and offer potential in next generation robotics and smart systems. This review specifically focuses on hydrogel‐based MAMs because of their mechanical compliance, programmability, biocompatibility, and cost‐efficiency. First, the composition of hydrogel MAMs along with the top‐down and bottom‐up approaches used for programming these materials are discussed. Next, the fundamental principles for engineering responsivity in MAMS, which includes optical, thermal, magnetic, electrical, chemical, and mechanical stimuli, are considered. Some advantages and disadvantages of different responsivities are compared. Then, to conclude, the emerging applications of hydrogel‐based MAMs from recently published literature, as well as the future outlook of MAM studies, are summarized.