Nanograting and Micro‐Protrusions Synergistic Dielectric Responses in Flexible Pressure Sensors for Ultrawide‐Range Human–Machine Perception

ABSTRACT Simultaneously achieving high sensitivity and a broad sensing range remains a fundamental challenge for flexible capacitive pressure sensors. Herein, we report a synergistic multiscale architecture featuring a polydimethylsiloxane/multi‐walled carbon nanotube nanocomposite dielectric, asymmetrically patterned with nanogratings and irregular micro‐protrusions, paired with an electrospun thermoplastic polyurethane nanofibrous network acting as an elastic buffer. By decoupling stress distribution mechanisms, this hierarchical design optimizes performance across all pressure regimes. At low pressures, the nanogratings induce severe localized stress to rapidly activate the percolation effect, maximizing initial sensitivity. Conversely, at high pressures, the micro‐protrusions and TPU layer progressively redistribute stress, effectively delaying mechanical saturation. Consequently, the sensor delivers an ultrahigh initial sensitivity of 12.34 kPa −1 across a broad 200 kPa working range, alongside rapid response (<30 ms) and robust durability (>5000 cycles). Demonstrating exceptional versatility in precise joint kinematic tracking, robotic grasping, and spatial pressure mapping, this structural engineering strategy establishes a compelling paradigm for next‐generation flexible sensors in smart healthcare and human–machine interfaces.