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Abstract Flexible piezoresistive‐sensing materials with high sensitivity and stable sensing signals are highly required to meet the accurate detecting requirement for human motion. Herein, a conductive poly(3,4‐ethylenedioxythiophene): poly(styrenesulfonate) / polydimethylsiloxane foam (P:P@p‐PSF) composite with strong interfacial action is designed. The porous structures and good interface combination not only show outstanding mechanical flexibility and reliability but also possess high sensitivity at a relatively wide strain range. The P:P@p‐PSF sensor achieves extreme sensitivity (Gauge Factor) of 6.25 in the subtle strain range of 1%–8%. Furthermore, the sensor forms a highly interconnected conductive network induced by the serious deformation of elastic‐interconnect pores, thus providing extremely sensitive sensing behavior for a relatively wide strain range (97.4% resistance change rate at 60% compressive strain). Moreover, the sensor presents repeatable stability and good thermal adaptation, which would meet the critical requirements of subtle vital signs, human motion monitoring, and so on. This work supplies insight into the design of a new flexible sensor material to overcome the weak interface problem and the flexible mismatch between conductive filler and matrix, showing great application potential in the field of electronic skin.

Advanced organic vapor sensors that simultaneously have high sensitivity, fast response, and good reproducibility are required. Herein, flexible, robust, and conductive vapor-grown carbon fibers (VGCFs)-filled polydimethylsiloxane (PDMS) porous composites (VGCFs/PDMS sponge (CPS)) with multilevel pores and thin, rough, and hollows wall were prepared based on the sacrificial template method and a simple dip-spin-coating process. The optimized material showed outstanding mechanical elasticity and durability, good electrical conductivity and hydrophobicity, as well as excellent acid and alkali tolerance. Additionally, CPS exhibited good reproducible sensing behavior, with a high sensitivity of ~1.5 × 105 s−1 for both static and flowing organic vapor, which was not affected in cases such as 20% squeezing deformation or environment humidity distraction (20~60% RH). Interestingly, both the reproducibility and sensitivity of CPS were better than those of film-shaped VGCFs/PDMS (CP), which has a thickness of two hundred microns. Therefore, the contradiction between the reproducibility and high sensitivity was well-solved here. The above excellent performance could be ascribed to the unique porous structures and the rough, thin, hollow wall of CPS, providing various gas channels and large contact areas for organic vapor penetration and diffusion. This work paves a new way for developing advanced vapor sensors by optimizing and tailoring the pore structure.