A paradigm-shifting design strategy is demonstrated that unifies the treatment of electronic and conformational properties of polymer dielectrics for concurrent high electric field and elevated temperature harsh conditions.

Due to their electrically polarized air‐filled internal pores, optimized ferroelectrets exhibit a remarkable piezoelectric response, making them suitable for energy harvesting. Expanded polytetrafluoroethylene (ePTFE) ferroelectret films are laminated with two fluorinated‐ethylene‐propylene (FEP) copolymer films and internally polarized by corona discharge. Poly(3,4‐ethylenedioxythiophene):poly(styrene sulfonate) (PEDOT:PSS)‐coated spandex fabric is employed for the electrodes to assemble an all‐organic ferroelectret nanogenerator (FENG). The outer electret‐plus‐electrode double layers form active device layers with deformable electric dipoles that strongly contribute to the overall piezoelectric response in the proposed concept of wearable nanogenerators. Thus, the FENG with spandex electrodes generates a short‐circuit current which is twice as high as that with aluminum electrodes. The stacking sequence spandex/FEP/ePTFE/FEP/ePTFE/FEP/spandex with an average pore size of 3 µm in the ePTFE films yields the best overall performance, which is also demonstrated by the displacement‐versus‐electric‐field loop results. The all‐organic FENGs are stable up to 90 °C and still perform well 9 months after being polarized. An optimized FENG makes three light emitting diodes (LEDs) blink twice with the energy generated during a single footstep. The new all‐organic FENG can thus continuously power wearable electronic devices and is easily integrated, for example, with clothing, other textiles, or shoe insoles.

Flexible large bandgap dielectric materials exhibiting ultra-fast charging-discharging rates are key components for electrification under extremely high electric fields. A polyoxafluoronorbornene (m-POFNB) with fused five-membered rings separated by alkenes and flexible single bonds as the backbone, rather than conjugated aromatic structure typically for conventional high-temperature polymers, is designed to achieve simultaneously high thermal stability and large bandgap. In addition, an asymmetrically fluorinated aromatic pendant group extended from the fused bicyclic structure of the backbone imparts m-POFNB with enhanced dipolar relaxation and thus high dielectric constant without sacrificing the bandgap. m-POFNB thereby exhibits an unprecedentedly high discharged energy density of 7.44 J/cm3 and high efficiency at 150 °C. This work points to a strategy to break the paradox of mutually exclusive constraints between bandgap, dielectric constant, and thermal stability in the design of all-organic polymer dielectrics for harsh condition electrifications.

Reconfigurable morphing surfaces provide new opportunities for advanced human-machine interfaces and bio-inspired robotics. Morphing into arbitrary surfaces on demand requires a device with a sufficiently large number of actuators and an inverse control strategy. Developing compact, efficient control interfaces and algorithms is vital for broader adoption. In this work, we describe a passively addressed robotic morphing surface (PARMS) composed of matrix-arranged ionic actuators. To reduce the complexity of the physical control interface, we introduce passive matrix addressing. Matrix addressing allows the control of N 2 independent actuators using only 2 N control inputs, which is substantially lower than traditional direct addressing ( N 2 control inputs). Using machine learning with finite element simulations for training, our control algorithm enables real-time, high-precision forward and inverse control, allowing PARMS to dynamically morph into arbitrary achievable predefined surfaces on demand. These innovations may enable the future implementation of PARMS in wearables, haptics, and augmented reality/virtual reality.

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