Electronic textiles and functional fabrics are among the key constituents envisioned for wearable electronics applications. For e‐textiles, the challenge is to process materials of desired electronic properties such as piezoelectricity into fibers to be integrated as wefts or wraps in the fabrics. Nylons, first introduced in the 1940s for stockings, are among the most widely used synthetic fibers in textiles. However, realization of nylon‐based e‐textiles has remained elusive due to the difficulty of achieving the piezoelectric phase in the nylon fibers. Here, piezoelectric nylon‐11 fibers are demonstrated and it is shown that the resulting fibers are viable for applications in energy harvesting from low frequency mechanical vibrations and in motion sensors. A simulation study is presented that elucidates on the sensitivity of the nylon‐11 fibers toward external mechanical stimuli. Moreover, a strategy is proposed and validated to significantly boost the electrical performance of the fibers. Since a large fraction of the textile industry is based on nylon fibers, the demonstration of piezoelectric nylon fibers will be a major step toward realization of electronic textiles for applications in apparels, health monitoring, sportswear, and portable energy generation.

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Ferroelectricity, a bistable ordering of electrical dipoles in a material, is widely used in sensors, actuators, nonlinear optics, and data storage. Traditional ferroelectrics are ceramic based. Ferroelectric polymers are inexpensive lead-free materials that offer unique features such as the freedom of design enabled by chemistry, the facile solution-based low-temperature processing, and mechanical flexibility. Among engineering polymers, odd nylons are ferroelectric. Since the discovery of ferroelectricity in polymers, nearly half a century ago, a solution-processed ferroelectric nylon thin film has not been demonstrated because of the strong tendency of nylon chains to form hydrogen bonds. We show the solution processing of transparent ferroelectric thin film capacitors of odd nylons. The demonstration of ferroelectricity, as well as the way to obtain thin films, makes odd nylons attractive for applications in flexible devices, soft robotics, biomedical devices, and electronic textiles.

Hierarchically porous piezoelectric polymer nanofibers are prepared through precise control over the thermodynamics and kinetics of liquid–liquid phase separation of nonsolvent (water) in poly(vinylidene fluoride‐trifluoroethylene) (P(VDF‐TrFE)) solution. Hierarchy is achieved by fabricating fibers with pores only on the surface of the fiber, or pores only inside the fiber with a closed surface, or pores that are homogeneously distributed in both the volume and surface of the nanofiber. For the fabrication of hierarchically porous nanofibers, guidelines are formulated. A detailed experimental and simulation study of the influence of different porosities on the electrical output of piezoelectric nanogenerators is presented. It is shown that bulk porosity significantly increases the power output of the comprising nanogenerator, whereas surface porosity deteriorates electrical performance. Finite element method simulations attribute the better performance to increased volumetric strain in bulk porous nanofibers.