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High‐performance and temperature‐resistant lithium‐ion batteries (LIBs), which are able to operate at elevated temperatures (i.e., >60 °C) are highly demanded in various fields, especially in military or aerospace exploration. However, their applications were largely impeded by the poor electrochemical performance and unsatisfying safety issues, which were induced by the severe side reactions between electrolytes and electrodes at high temperatures. Herein, with the synergetic effects of solvation chemistry and functional additive in the elaborately designed weakly solvating electrolyte, a unique robust organic/inorganic hetero‐interphase, composed of gradient F, B‐rich inorganic components and homogeneously distributed Si‐rich organic components, was successfully constructed on both cathodes and anodes, which would effectively inhibit the constant decomposition of electrolytes and dissolution of transition metal ions, thus highly enhancing the high‐temperature electrochemical performance. As a result, both cathodes and anodes, without compromising their low‐temperature performance, can operate at temperatures ≥100 °C, with excellent capacity retentions of 96.1 % after 500 cycles and 93.5 % after ≥200 cycles, respectively, at 80 °C. Ah‐level LiCoO2||graphite full cells with a cut‐off voltage of 4.3 V also exhibited superior temperature‐resistance with a capacity retention of 89.9 % at temperature as high as 120 °C. Moreover, the fully charged pouch cells exhibited highly enhanced safety, demonstrating their potentials in practical applications at ultrahigh temperatures. [ABSTRACT FROM AUTHOR]

Aqueous zinc‐ion batteries (AZIBs) attract attention due to their safety and high specific capacity. However, their practical applications are constrained by Zn anode corrosion, dendritic growth, and poor temperature adaptability induced by a strong hydrogen‐bond network in aqueous electrolytes. Herein, a universal strategy to design strong solvating electrolytes is proposed, in which the hydrogen‐bond network and solvation structures are reconstructed by regulating the dipolar‐dipolar and ion‐dipolar interactions simultaneously. Consequently, the hydrogen‐bond network in free water is largely weakened, and the water content in the Zn2+ solvated sheath is reduced, while the hydrogen‐bond network between solvents is strengthened, which effectively broadens the operating temperature range and suppresses Zn dendrites and corrosion. As a result, Zn anodes exhibit excellent platting/stripping efficiency with an average Coulombic Efficiency up to 99.89% after 2000 cycles at 0.5 mA cm−2, impressive cycling stability (5000 h, 0.5 mA cm−2/0.5 mA h cm−2), and a wide operating temperature range of 140 °C (−50–90 °C). Moreover, the Zn//V2O3 full cells also display enhanced temperature‐resistance, implying that the designed strong solvation electrolyte has practical application potential in extreme environments. This study suggests a promising strategy to design ideal electrolytes for high‐performance AZIBs with safety, ultralong cycling life, and satisfying temperature‐resistance. [ABSTRACT FROM AUTHOR]