AbstractSoft‐ionic materials with biocompatibility and 3D printability are needed to develop next‐generation devices to interface between electronic and biological signals. Herein, thermoreversible and biocompatible ionic liquid gels or iongels, which can be processed by direct ink writing are reported. The iongels are designed by taking advantage of polyvinyl alcohol/phenol interactions to gelify biocompatible cholinium carboxylate ionic liquids. The obtained iongels are stable, soft, and flexible materials (Young modulus between 14 and 70 kPa) with high ionic conductivity (1.8 × 10–2 S cm–1). Interestingly, they presented thermoreversible properties with gel–sol transitions ranging from 85 and 110 °C, which allows the iongel processing via direct ink writing 3D printing by material extrusion at temperatures over its transition. These 3D printable iongels are integrated into a variety of body sensors applications, namely pressure sensors, motion sensors and electrodes for electrophysiological recordings. The iongels are used as pressure sensors with a sensitivity of 0.1 kPa–1, ten times higher than that of others similar materials reported so far; showing its ability to detect human motion. Furthermore, the iongels showed excellent performance in electrodes for electrocardiography (ECG) recording, presenting good stability over time with electrocardiographic waves maintained their typical shape even after weeks.
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