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 Ti₃C₂T_x 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 Ti₃C₂T_x 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 (Mg_1/3Nb_2/3)O₃-PbTiO₃/polyvinylidene fluoride composite nanofibers by 160% via Ti₃C₂T_x 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.

We report the sea sponge-inspired design and preparation of piezoelectric composite generators (PCGs) based on a three-dimensional electroceramic skeleton. The remarkable improvements in the piezopotential of the bioinspired structure have been theoretically analyzed using numerical simulations based on a phase-field simulation. The open-circuit voltage, short-circuit current density and instantaneous power density of the bioinspired PCG reach up to ∼25 V, ∼550 nA cm⁻² and ∼2.6 μW cm⁻², respectively, corresponding to about 16 times higher power than that of conventional particle based piezoelectric polymer composites. Moreover, the bioinspired PCG displays 30 times higher strain–voltage efficiency under stretching than the state-of-the-art performance of the flexible piezoelectric energy harvesters reported so far.

Exploring the dynamic responses of a material is of importance to both understanding its fundamental physics at high frequencies and potential device applications. Here we develop a phase-field model for predicting the dynamics of ferroelectric materials and study the dynamic responses of ferroelectric domains and domain walls subjected to an ultrafast electric-field pulse. We discover a transition of domain evolution mechanisms from pure domain growth at a relatively low field to combined nucleation and growth of domains at a high field. We derive analytical models for the two regimes which allow us to extract the effective mass and damping coefficient of ferroelectric domain walls. The exhibition of two regimes for the ferroelectric domain dynamics at low and high electric fields is expected to be a general phenomenon that would appear for ferroic domains under other ultrafast stimuli. The present Letter also offers a general framework for studying domain dynamics and obtaining fundamental properties of domain walls and thus for manipulating the dynamic functionalities of ferroelectric materials.