Tough and stretchable conductive hydrogels are desirable for the emerging field of wearable and implanted electronics. Unfortunately, most existing conductive hydrogels have low mechanical strength. Current strategies to enhance mechanical properties include employing tough host gel matrices or introducing specific interaction between conductive polymer and host gel matrices. However, these strategies often involve additional complicated processes. Here, a simple yet effective soaking treatment is employed to concurrently enhance mechanical and conductive properties, both of which can be facilely tailored by controlling the soaking duration. The significant improvements are correlated with co-occurring mechanism of deswelling and multiple noncovalent interactions. The resulting optimal sample exhibits attractive combination of high water content (75 wt %), high tensile stress (∼2.5 MPa), large elongation (>600%), reasonable conductivity (∼25 mS/cm), and fast self-healing property with the aid of hot water. The potential application of gel as a strain sensor is demonstrated. The applicability of this method is not limited to conductive hydrogels alone but can also be extended to strengthen other functional hydrogels with weak mechanical properties.

N-Alky-substituted carbamate-modified PVA as a layer material to enable multi-responsive, bidirectional and large deformation actuation.

Simple soaking treatment generates layered hydrogels with a combination of superior mechanics and chemical robustness.

This work reports a self-healing and shape-memory hydrogel integrating multiple mechanical properties. The network configuration is featured as entangled networks cross-linked by distributed association of very short alkyl chains (hexyl, six carbons). These cross-linking knots are interconnected by the long hydrophilic polyvinyl alcohol backbone. The optimal aggregation of hexyl side chains leads to the broadened distribution in bonding strength as verified by static and dynamic mechanical characterization. These structural features contribute to high strength, toughness, stiffness, and yet fast recoverability. Furthermore, the hydrophobic and supramolecular nature of aggregated alkyl chains offers high durability and solvent-assistant healing function. Finally, distributed association of hexyl side chains confers a broadened temperaturedependent modulus, allowing for encoding stepwise shape recovery from a temporary shape at different temperatures and/or times.

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