Thermoelectric generators (TEGs) are an excellent candidate for powering wearable electronics and the “Internet of Things,” due to their capability of directly converting heat to electrical energy. Here, we report a high-performance wearable TEG with superior stretchability, self-healability, recyclability, and Lego-like reconfigurability, by combining modular thermoelectric chips, dynamic covalent polyimine, and flowable liquid-metal electrical wiring in a mechanical architecture design of “soft motherboard-rigid plugin modules.” A record-high open-circuit voltage among flexible TEGs is achieved, reaching 1 V/cm2 at a temperature difference of 95 K. Furthermore, this TEG is integrated with a wavelength-selective metamaterial film on the cold side, leading to greatly improved device performance under solar irradiation, which is critically important for wearable energy harvesting during outdoor activities. The optimal properties and design concepts of TEGs reported here can pave the way for delivering the next-generation high-performance, adaptable, customizable, durable, economical, and eco-friendly energy-harvesting devices with wide applications.

Grain or phase boundaries play a critical role in the carrier and phonon transport in bulk thermoelectric materials. Previous investigations about controlling boundaries primarily focused on the reducing grain size or forming nanoinclusions. Herein, liquid phase compaction method is first used to fabricate the Yb‐filled CoSb3 with excess Sb content, which shows the typical feature of low‐angle grain boundaries with dense dislocation arrays. Seebeck coefficients show a dramatic increase via energy filtering effect through dislocation arrays with little deterioration on the carrier mobility, which significantly enhances the power factor over a broad temperature range with a high room‐temperature value around 47 μW cm−2 K−1. Simultaneously, the lattice thermal conductivity could be further suppressed via scattering phonons via dense dislocation scattering. As a result, the highest average figure of merit ZT of ≈1.08 from 300 to 850 K could be realized, comparable to the best reported result of single or triple‐filled Skutterudites. This work clearly points out that low‐angle grain boundaries fabricated by liquid phase compaction method could concurrently optimize the electrical and thermal transport properties leading to an obvious enhancement of both power factor and ZT.

A highly durable high-performance all-polymer micro-supercapacitor with plug-and-play function is developed. Through the newly developed technology, these micro-supercapacitors can be transferred to any substrate with all functions well retained.

Despite the unfavorable band structure with twofold degeneracy at the valence band maximum, MgAgSb is still an excellent p‐type thermoelectric material for applications near room temperature. The intrinsically weak electron–phonon coupling, reflected by the low deformation potential Edef ≈ 6.3 eV, plays a crucial role in the relatively high power factor of MgAgSb. More importantly, Li is successfully doped into Mg site to tune the carrier concentration, leading to the resistivity reduction by a factor of 3 and a consequent increase in power factor by ≈30% at 300 K. Low lattice thermal conductivity can be simultaneously achieved by all‐scale hierarchical phonon scattering architecture including high density of dislocations and nanoscale stacking faults, nanoinclusions, and multiscale grain boundaries. Collectively, much higher average power factor ≈25 μW cm−1 K−2 with a high average ZT ≈ 1.1 from 300 to 548 K is achieved for 0.01 Li doping, which would result in a high output power density ≈1.56 W cm−2 and leg efficiency ≈9.2% by calculations assuming cold‐side temperature Tc = 323 K, hot‐side temperature Th = 548 K, and leg length = 2 mm.

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