High-fidelity wireless electrophysiological monitoring is essential for ambulatory healthcare applications. Soft solid-like hydrogels have received significant attention as epidermal electrodes because of their tissue-like mechanical properties and high biocompatibility. However, it is challenging to develop a hydrogel electrode that provides robust contact and high adhesiveness with glabrous skin and hairy scalp for high-fidelity, continuous electrophysiological signal detection. Here, a paintable, fast gelation, highly adhesive, and conductive hydrogel is engineered for high-fidelity wireless electrophysiological monitoring. The hydrogel, consisting of gelatin, gallic acid, sodium citrate, lithium chloride, glycerol, and Tris-HCl buffer solution exhibits a reversible thermal phase transition capability, which endows it with the attributes of on-skin applicability and fast in situ gelation with 15 s, thereby addressing the aforementioned limitations. The introduction of gallic acid enhances the adhesive properties of the hydrogel, facilitating secure electrode attachment to the skin or hairy scalp. To accentuate the potential applications in at-home electrophysiological health monitoring, the hydrogel electrodes are demonstrated for high-fidelity electrocardiogram recording for one hour during various daily activities, as well as in simultaneous electroencephalogram and electrocardiogram recording during a 30 min nap.
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