Ankan Dutta, Md Abu Sayeed Biswas, Ethan Gerhard, Mayukh Das, Long Meng, Wanqing Zhang, W C Winnie Li, Arantza Moreno Calva, Shakul Pathak, Jie Yang, Junyi Yin, Jordan Meyet, Shuvendu Das, Bed Poudel, Abu Musa Abdullah, Yuju Che, Cheng‐Hsin Chuang, Jie Yang, Sihong Wang, Xiaogang Hu, Saptarshi Das, Huanyu Cheng
Integrating thermoreversibility with electrical conductivity in a unified hydrogel platform enables long-term, reusable through-hair neural interfaces. However, achieving both simultaneously remains challenging, as thermoreversibility demands network reorganization while conductivity necessitates network percolation. Here, we engineer phase morphology by controlling the components’ viscoelastic state during mixing. Ionically conductive nucleated morphologies illustrated by liquid-liquid phase separation exhibit rapid thermoreversibility, whereas electrically conductive bicontinuous phases demonstrated by viscoelastic phase separation achieve a marginal gel-sol transition and an ultralow storage modulus of ~1.7 kilopascals while simultaneously achieving a conductivity of 7.5 siemens per centimeter or transconductance of 5.1 millisiemens in an organic electrochemical transistor. Below this threshold, systems resemble nucleated behavior, whereas above it, superior semiconducting properties emerge, but phase transition capability is lost. These materials enable reusable through-hair neural interfaces to maintain low skin contact impedance of 1.6 kohm·cm 2 across different hair types for 3 days, facilitating stable event-related desynchronization detection during mechanical and electrical haptic sensation for personalized haptics.