Cyclic Pulsating Pressure–Induced Structural Evolution and Interfacial Coupling in TPU / CNT Composites

ABSTRACT Flexible strain sensors hold great potential for wearable electronics, electronic skin, and intelligent human–machine interfaces, but achieving both high sensitivity and sufficient stretchability under repeated deformations remains a critical challenge. Here, we present a cyclic pulsating pressure molding strategy that enables the formation of a dense and stable conductive network while reinforcing interfacial coupling. This approach markedly enhances the composite performance, yielding an electrical conductivity of 0.41 S·cm −1 and an elongation at break of 256%, corresponding to increases of 64% and 34.7% compared with conventional constant‐pressure molded samples. Under strains up to 256%, the sensor delivers a relative resistance change of 4.8 × 10 4 % (GF ≈ 550). It also maintains signal fluctuations within ±5% after 1000 cycles at 1% strain and achieves high‐fidelity strain detection across complex motion states, demonstrating reliable cyclic stability and adaptability. Overall, cyclic pulsating pressure processing offers a simple and universal route to high‐performance flexible resistive strain sensors and provides a pathway for their scalable application in wearable electronics, electronic skin, and human–machine interfaces.