Anisotropic Nanofiber Architectures for Strain‐Insensitive Pressure Sensing and Stretchable Interconnects

ABSTRACT The rapid advancement of flexible electronics demands materials that combine mechanical compliance, operational stability, and reliable functionality under dynamic mechanical stresses. Here, we report electrospun poly(3,4‐ethylenedioxythiophene):polystyrenesulfonate (PEDOT:PSS)/polyacrylamide (PAAm) nanofiber mats as robust active components for next‐generation stretchable bioelectronics. Characterized by a hierarchical porous architecture, these mats facilitate efficient charge transport while offering superior mechanical resilience compared to conventional hydrogels or brittle thin films. Mechanical investigations reveal pronounced electromechanical anisotropy: the mats maintain minimal resistance variation under tensile strain, attributed to reversible fiber realignment within the interconnected nanofiber network, yet exhibit high sensitivity to compressive stress associated with structural perturbation within the porous conductive network. This intrinsic directional selectivity may be advantageous for pressure‐sensitive tactile sensing while minimizing signal variations arising from bending or stretching deformation. Furthermore, when integrated into flexible interconnects and mounted on human joints, the mats demonstrate stable electrical response under physiological deformations, as verified by in situ resistance monitoring. These results establish PEDOT:PSS/PAAm nanofiber mats as mechanically stable and direction‐sensitive building blocks for pressure‐selective wearable sensing and soft robotic applications.