Non-wetting and Conductive Janus Structure for High-Performance Electronics Enabled by Gradient Polarity Driven Hierarchical Spatial Assembly

Achieving simultaneous high conductivity and water repellency in flexible polymer composites remains a fundamental challenge for wearable sensors, because conventional hydrophobic coatings introduce thick insulating layers that degrade electrical performance. Here, we present a gradient polarity-mediated self-assembly strategy to fabricate Janus-structured nanocomposites (Janus-HC-NW) that spatially decouple conductivity and non-wettability. The design features a topographical layer of VTES@TiO ₂ sub-microscale agglomerates for stabilizing air-entrapping triple-phase interfaces (contact angle of 154.1°), while a bottom layer of monodispersed MWCNT with ultrathin VTES coatings (~ 34 nm) ensures unimpeded charge transport. Density functional theory reveals TiO ₂ ’s critical role in regulating VTES distribution via preferential Si-O-Ti bonding (-3.12 eV vs. -1.84 eV for VTES@MWCNT), enabling nanoscale control over polymer encapsulation. The Janus-HC-NW exhibits a 77-fold conductivity enhancement and exceptional environmental stability. Integrated into wood sponge-based sensors, it achieves a 12.4-fold sensitivity increase, 6.93-fold higher signal-to-noise ratio, and 4.95-fold improved electromagnetic shielding, enabling precise underwater micro-vibration detection in harsh conditions. This work would establish a paradigm for multifunctional composites in next-generation flexible electronics.