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The electrolyte carbonation and the resulting air electrode plugging are the primary factors limiting the cycle life of aqueous alkaline zinc–air batteries (ZABs). In this work, calcium ion (Ca2+) additives were introduced into the electrolyte and the separator to resolve the above issues. Galvanostatic charge–discharge cycle tests were carried out to verify the effect of Ca2+ on electrolyte carbonation. With the modified electrolyte and separator, the cycle life of ZABs was improved by 22.2% and 24.7%, respectively. Ca2+ was introduced into the ZAB system to preferentially react with CO32− rather than K+ and then precipitated granular CaCO3 prior to K2CO3, which was deposited on the surface of the Zn anode and air cathode to form a flower-like CaCO3 layer, thereby prolonging its cycle life.