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HighlightsThe ratio of hydrogen bonds in water molecules is significantly decreased by introducing oxygen-ligand Mg 2+  and hydrogen-ligand ClO 4 −, resulting in an ultralow solidifying point of − 121 °C.    The excellent low-temperature physicochemical properties and good compatibility with Zn metal of 3.5 M (mol L −1 ) Mg(ClO 4 ) 2  + 1 M Zn(ClO 4 ) 2  electrolyte gives fabricated Zn||pyrene-4,5,9,10-tetraone (PTO) battery and Zn||Phenazine (PNZ) battery a satisfactory low temperature performance.Supplementary Information  The online version contains supplementary material available at 10.1007/s40820-021-00733-0.

Synergistic Effect of Cation and Anion for Low-Temperature Aqueous Zinc-Ion Battery