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Exploitation of soft piezoelectric sensing materials is fundamental to the research of energy‐harvesting devices and wearable electronics. However, a big challenge of piezoelectric materials application in micro‐scale sensing systems is to address the restrictions of electrode compatibility, miniaturization, multistep assembly, and high cost. Here, we propose a simple strategy to develop the coinstantaneous construction of piezoelectric materials and nanoresistance networks by fabricating electrospun piezoelectric‐conductive (polyacrylonitrile)//(polyaniline/polyvinyl pyrrolidone) (denoted [PAN]//[PANI/PVP]) Janus nanofibers (NFs). This peculiar Janus structure can collect and output voltage by conductive paths based on the Wheatstone bridge principle. Moreover, owing to the nanoscale asymmetric geometry for efficient polarization and induced charges collection, the Janus NFs show superior piezoelectric properties. As a result, flexible (PAN)//(PANI/PVP) Janus nanofibers integrated membrane (JNFIM) dispensing with two flat electrodes can directly output a high voltage of 2 V under a tiny force of 1 N. Furthermore, the JNFIM enables to detect pressures with extra‐high linear sensitivity (1.88 V N−1) and low detection limit (0.1 N). Thus, our work provides a simple route for the development of nanoscale, low‐cost, and high‐sensitivity integrated materials for pressure sensing, revealing promising applications in miniature robotics and wearable devices.

Fabrication of flexible piezoelectric sensing nanomaterials is essential for the development of wearable and microscopic electronic devices. However, existing piezoelectric sensing materials usually rely on the secondary synthesis process to accomplish the preparation of conductive layer electrodes. Here, we report a one-step strategy for synchronous construction of piezoelectric elements and nanoresistance networks via fabricating flexible [polyacrylonitrile/BaTiO3]@[polyaniline/polyvinyl pyrrolidone] core–shell nanofibers (NFs, denoted [PAN/BTO]@[PANI/PVP]) by coaxial electrospinning. This is the first time to collect and output voltage signals generated by piezoelectric materials through nanoresistance networks based on the Wheatstone bridge principle. As a result, flexible [PAN/BTO]@[PANI/PVP] core–shell NFs as an integrated sensing system without layer electrodes can directly result in voltage signals under repeating press–release motions. The potential of a flexible core–shell [PAN/BTO]@[PANI/PVP] integrated nanofiber membrane (INFM) for pressure sensing is properly explored and evaluated. The integration of piezoelectric elements and nanoresistance networks enables the INFM to perceive pressures with high sensitivity (728 mV N–1) down to approximately 0.05 N and a quick response (26 ms). Overall, our study demonstrates a promising strategy to fabricate nanoscale, highly sensitive, and low-cost integrated sensing materials, which have potential applications in micro-/nanoscale sensors and wearable electronics.

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