Zinc-air batteries (ZABs) using gel polymer electrolytes suffer from low energy efficiency and poor cyclability. This issue is not only associated with the air electrode, as early failure of the battery is often due to the Zn electrode. Here, the cycle life of ZABs using alkaline poly(acrylic acid) (PAA-KOH) as the electrolyte is shown to vary by changing its crosslinking density. For ZABs using hydrogel electrolytes, understanding the failure mechanism and optimization of the hydrogel composition are key to achieving better utilization of the Zn electrode and battery rechargeability. In addition, the effects of crosslinker concentration on rheological properties, sol-gel fraction, ionic conductivity, and water retention ability of the hydrogel are discussed. PAA-KOH gels with lower crosslinking concentrations are weaker, but they have higher conductivity and better water retention, whereas gels with higher crosslinking concentrations affect the diffusion of zincate ions and facilitate passivation of the Zn electrode, resulting in early failure of the battery.[a] T.