AbstractSurface electrodes monitoring various electrophysiological activities with high sensitivity are crucial for studying electrical phenomena in living organisms. However, the sensitivity of current surface electrodes is limited due to electron transmission losses and signal attenuation at the electrode‐skin interface. Here, a bicontinuous liquid metal/polymer film electrode is developed, in which up to 92 wt.% of liquid metal is stably immobilized within a 3D continuous polymer network via electrostatic interactions. This electrode facilitates fast electron transport, enhances skin adhesion through hydrogen bonding, and ensures conformal contact due to its flexibility. As a result, the electrode achieves a sensitivity of 20 µV N−1, representing an improvement of 400% over the highest performance reported to date. This leap in sensitivity enables the high‐resolution monitoring of electrophysiological signals, allowing for earlier and more accurate identification of myocardial infarction abnormalities. Moreover, this high‐sensitivity electrode has the potential to develop an intelligent sensory system for material recognition and provide real‐time warnings in hazardous situations for individuals with tactile impairments.
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