Ultra‐Tough Graphene Oxide/DNA 2D Hydrogel with Intrinsic Sensing and Actuation Functions

Hydrogel devices with mechanical toughness and tunable functionalities are highly desirable for practical long‐term applications such as sensing and actuation elements for soft robotics. However, existing hydrogels have poor mechanical properties, slow rates of response, and low functionality. In this work, two‐dimensional hydrogel actuators are proposed and formed on the self‐assembly of graphene oxide (GO) and deoxynucleic acid (DNA). The self‐assembly process is driven by the GO‐induced transition of double stranded DNA (dsDNA) into single stranded DNA (ssDNA). Thus, the hydrogel's structural unit consists of two layers of GO covered by ssDNA and a layer of dsDNA in between. Such heterogeneous architectures stabilized by multiple hydrogen bondings have Young's modulus of up to 10 GPa and rapid swelling rates of 4.0 × 10 −3 to 1.1 × 10 −2 s −1 , which surpasses most types of conventional hydrogels. It is demonstrated that the GO/DNA hydrogel actuators leverage the unique properties of these two materials, making them excellent candidates for various applications requiring sensing and actuation functions, such as artificial skin, wearable electronics, bioelectronics, and drug delivery systems.