Flexible and highly sensitive pressure sensors have versatile biomedical engineering applications for disease diagnosis and healthcare. The fabrication of such sensors based on porous structure composites usually requires complex, costly, and nonenvironmentally friendly procedures. As such, it is highly desired to develop facile, economical, and environment‐friendly fabrication strategies for highly sensitive lightweight pressure sensors. Herein, a novel design strategy is reported to fabricate porous composite pressure sensors via a simple heat molding of conductive fillers and thermoplastic polyurethane (TPU) powders together with commercially available popcorn salts followed by water‐assisted salt removal. The obtained TPU/carbon nanostructure (CNS) foam sensors have a linear resistance response up to 60% compressive strain with a gauge factor (GF) of 1.5 and show reversible and reproducible piezoresistive properties due to the robust electrically conductive pathways formed on the foam struts. Such foam sensors can be potentially utilized for guiding squatting exercises and respiration rate monitoring in daily physical training.

Simultaneously achieving high piezoresistive sensitivity, stretchability, and good electrical conductivity in conductive elastomer composites (CECs) with carbon nanofillers is crucial for stretchable strain sensor and electrode applications. Here, we report a facile and environmentally friendly strategy to realize these three goals at once by using branched carbon nanotubes, also known as the carbon nanostructure (CNS). Inspired by the brick-wall structure, a robust segregated conductive network of a CNS is formed in the thermoplastic polyurethane (TPU) matrix at a very low filler fraction, which renders the composite very good electrical, mechanical, and piezoresistive properties. An extremely low percolation threshold of 0.06 wt %, currently the lowest for TPU-based CECs, is achieved via this strategy. Meanwhile, the electrical conductivity is up to 1 and 40 S/m for the composites with 0.7 and 4 wt % CNS, respectively. Tunable piezoresistive sensitivity dependent on CNS content is obtained, and the composite with 0.7 wt % filler has a gauge factor up to 6861 at strain ε = 660% (elongation at break is 950%). In addition, this strategy also renders the composites’ attractive tensile modulus. The composite with 3 wt % CNS shows 450% improvement in Young’s modulus versus neat TPU. This work introduces a facile strategy to fabricate highly stretchable strain sensors by designing CNS network structures, advancing understanding of the effects of polymer–filler interfaces on the mechanical and electrical property enhancements for polymer nanocomposites.

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Carbon nanofiller dimensionality affects the morphology of conductive networks built via an interface engineering strategy in composite materials, enabling the design of different flexible sensors and conductors for electronic applications.