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Inorganic solid electrolytes offer inherently unique transport, thermal, and mechanical attributes that can potentially address the fast‐charging barriers of safety, performance, and degradation exhibited by their liquid counterparts; however, to achieve reliable fast charging while retaining long cycle life remains a challenge for all‐solid‐state lithium batteries (ASSLBs), which is hindered by the electro‐chemo‐mechanical and transport issues at solid–solid interface. Herein, a high‐entropy strategy is reported to design ideal argyrodite electrolytes for fast‐charging ASSLBs with boosted transport kinetics and mitigated electrolyte‐electrode reactions via anionic site disordering. As proof of concept, multiple aliovalent cations (Si4+/Ge4+/Sn4+) and anions (Cl−) are introduced to Li6PS5Br (LPSBr) to prepare its high‐entropy counterpart, HE‐LPSBrCl. As the configuration entropy increases from 1.35 to 2.29 R, the disordering increases by 6.83‐fold and ionic conductivity increases by nearly one order of magnitude (7.96 mS cm−1 at 30 °C for HE‐LPSBrCl). The HE‐LPSBrCl full cells deliver a high capacity of 67.7 mA h g−1 at 10 C, 61.5 times higher than that of LPSBr counterparts, and retain 85.6% of the capacity (96.2 mA h g−1 at 5 C) after 1400 cycles. Unwanted mechanical penetration of Li and interfacial delamination and particle cracking of composite cathode at high rates are successfully suppressed. [ABSTRACT FROM AUTHOR]

Piezoelectric polarization portrays a promising technology to regulate the photogenerated charge carrier separation and transfer behaviors, and the design of multifunctional catalysts with piezo‐phototronic effect is a key step. One strategy is to prepare a composite catalyst combining the ideal properties from each individual component. Herein, a facial dopant‐induced self‐assembling strategy is reported to fabricate an ultracompact nanocomposite (LaFeO3/ZnFe2O4/La2O3) with enhanced efficiency for piezo‐photocatalysis. The composite is synthesized at 800 °C from the one‐pot method, thus the self‐constructed interface is created during multi‐phase formation, providing the intimate grain‐to‐grain contact between the semiconductive LaFeO3 and piezoelectric ZnFe2O4/La2O3 phases. In such a composite, a synergistic effect for oxygen activation is realized via the effective manipulation of the photogenerated charge carrier separation and spatial transportation through the vibration‐created piezopotential. A high piezoelectric coefficient (d33) up to 826 pm V−1 and a superior H2O2 yield of 403 µmol g−1 h−1 (in open air and pure water) are achieved on the optimized composite, outperforming most of the reported lead‐free piezo‐photocatalyst. The ultracompact composite is very robust without any decay in H2O2‐delivering capability after many cyclic tests. This study provides a universal strategy for the rational design of high‐performance piezo‐photocatalysts. [ABSTRACT FROM AUTHOR]