The development of multifunctional electromagnetic interference (EMI) shielding materials has garnered significant attention, yet achieving flexible composites that integrate EMI shielding, thermal conductivity, and other functionalities under low filler loading remains a challenge. This study presents a novel flexible composite with segregated structure prepared via a simple co-mixing and hot-pressing method. By selectively distributing conductive Liquid metal (LM) and Multi-wall carbon nanotube (CNT) on the surface of Polyurethane (TPU) particles, a continuous and compact conductive network is successfully constructed, enabling the attainment of a high EMI shielding effectiveness of 80.2 dB and a thermal conductivity of 4.8 W m−1 K−1 even at low LM loadings. Furthermore, the composite exhibits low-voltage-driven Joule heating performance, excellent photothermal conversion efficiency, and promising potential for wearable sensor applications. The combination of these outstanding properties highlights the great potential of LM-based composites for next-generation wearable devices.
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