In non-ionic conductive hydrogels, conductivity often conflicts with mechanical properties, posing a challenge in creating hydrogels that strike a balance between conductivity and mechanical properties. Here, we addressed this issue by integrating carboxylated carbon nanotube (CNT) layers in a sandwich structure onto the surface of the cationic hydrogel (P(AM-co-DMDAAC), PAD), followed by dehydration for densification. This approach simultaneously improved the conductivity of the hydrogel while maintaining its stretchability. The stability of the composite structure was ensured through electrostatic interactions, hydrogen bonding, and physical entanglement between the PAD hydrogel and the CNT layer. Additionally, adjusting the water–solid ratio of the hydrogel allows fine-tuning of its conductivity and stretchability. Remarkably, at a 500 % water–solid ratio, the hydrogel achieved a conductivity of 2.3 S/m. By further reducing the water content, the conductivity could be increased to 25 S/m, significantly higher than similar hydrogels. The PAD-CNT hydrogel found applications in swelling response, tunable resistance wires, and as strain sensors. Notably, the sandwich structure enables the PAD-CNT hydrogel to output capacitive signals, exhibiting a more sensitive response in monitoring human movement. Overall, this study introduces a novel composite structure for conductive hydrogels, holding tremendous potential in flexible conductivity and smart response fields.
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