The next‐generation wearable biosensors with highly biocompatible, stretchable, and robust features are expected to enable the change of the current reactive and disease‐centric healthcare system to a personalized model with a focus on disease prevention and health promotion. Herein, a muscle‐fiber‐inspired nonwoven piezoelectric textile with tunable mechanical properties for wearable physiological monitoring is developed. To mimic the muscle fibers, polydopamine (PDA) is dispersed into the electrospun barium titanate/polyvinylidene fluoride (BTO/PVDF) nanofibers to enhance the interfacial‐adhesion, mechanical strength, and piezoelectric properties. Such improvements are both experimentally observed via mechanical characterization and theoretically verified by the phase‐field simulation. Taking the PDA@BTO/PVDF nanofibers as the building blocks, a nonwoven light‐weight piezoelectric textile is fabricated, which hold an outstanding sensitivity (3.95 V N−1) and long‐term stability (<3% decline after 7,400 cycles). The piezoelectric textile demonstrates multiple potential applications, including pulse wave measurement, human motion monitoring, and active voice recognition. By creatively mimicking the muscle fibers, this work paves a cost‐effective way to develop high‐performance and self‐powered wearable bioelectronics for personalized healthcare.

Polymer-ceramic piezoelectric composites, combining high piezoelectricity and mechanical flexibility, have attracted increasing interest in both academia and industry. However, their piezoelectric activity is largely limited by intrinsically low crystallinity and weak spontaneous polarization. Here, we propose a Ti3C2Tx MXene anchoring method to manipulate the intermolecular interactions within the all-trans conformation of a polymer matrix. Employing phase-field simulation and molecular dynamics calculations, we show that OH surface terminations on the Ti3C2Tx nanosheets offer hydrogen bonding with the fluoropolymer matrix, leading to dipole alignment and enhanced net spontaneous polarization of the polymer-ceramic composites. We then translated this interfacial bonding strategy into electrospinning to boost the piezoelectric response of samarium doped Pb (Mg1/3Nb2/3)O3-PbTiO3/polyvinylidene fluoride composite nanofibers by 160% via Ti3C2Tx nanosheets inclusion. With excellent piezoelectric and mechanical attributes, the as-electrospun piezoelectric nanofibers can be easily integrated into the conventional shoe insoles to form a foot sensor network for all-around gait patterns monitoring, walking habits identification and Metatarsalgi prognosis. This work utilizes the interfacial coupling mechanism of intermolecular anchoring as a strategy to develop high-performance piezoelectric composites for wearable electronics.

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