Phase Separation Manipulated Gradient Conductivity for A High‐Precision Flexible Pressure Sensor

Abstract Piezoresistive pressure sensors, analyzing and converting external pressure signals to readable electrical signals for monitoring human health, are always subjected to simultaneously possess high signal‐linearity and signal sensitivity. Analogous to the control of sophisticated microstructure for increasing active sensing area, the control of gradient conductivity should enable a linear response via regulating the formed saturation current. Here, inspired by phase separation showing the feasibility of controlling material microstructure and conductivity, a high‐performance flexible pressure sensor via the simultaneous control of microgroove structure and wide‐range gradient conductivity is demonstrated. First, a laser‐etching and dopamine (DA)‐doping synergistic approach is used to induce selective phase separation in poly(3,4‐ethylenedioxythiophene): poly(styrenesulfonic acid) (PEDOT:PSS), achieving broad conductivity modulation (from 297 to 4525 S cm⁻¹) and precise microgroove pattern (15.5 µm). Then, by designing conductivity‐gradient PEDOT: PSS‐based multi‐sublayers and microgroove interlocked structure, the sensor shows extraordinarily comprehensive performance of excellent stress‐sensing sensitivity (4 × 10⁵ kPa⁻¹), high linear responsiveness (99.85%) and wide‐range sensing ability (up to 100 kPa). Consequently, this sensor reveals excellent capability in detecting multi‐mode pressure changes and is expected to branch out into other electronic device designs as a general strategy for the precise manipulation of material physical‐chemical properties.