Due to the slow dynamics of mass and charge transfer at Zn|electrolyte interface, the stable operation of Zn–air batteries (ZABs) is challenging, especially at low temperature. Herein, inspired by cell membrane, a hydrophilic‐hydrophobic dual modulated Zn|electrolyte interface is constructed. This amphiphilic design enables the quasi‐solid‐state (QSS) ZABs to display a long‐term cyclability of 180 h@50 mA cm−2 at 25 °C. Moreover, a record‐long time of 173 h@4 mA cm−2 at −60 °C is also achieved, which is almost threefolds of untreated QSS ZABs. Control experiments and (in situ) characterization reveal that the growth of insulating ZnO passivation layers is largely inhibited by tuned hydrophilic–hydrophobic behavior. Thus, the enhanced transfer dynamic of Zn2+ at Zn|electrolyte interface from 25 to −60 °C is attained. As an extension, the QSS Al‐air batteries (AABs) with bioinspired interface also show unprecedented discharge stability of 420 h@1 mA cm−2 at ‐40 °C, which is about two times of untreated QSS AABs. This bioinspired‐hydrophilic‐hydrophobic dual modulation strategy may provide a reference for energy transform and storage devices with broad temperature adaptability.