The uneven flux and strong solvation of Zn²⁺ ions in aqueous electrolytes bring undesirable dendritic deposition and side reactions to zinc metal anodes (ZMAs). Hydrogel electrolytes have considerable mechanical strength and limited water content, which can suppress dendrite growth and alleviate side reactions. Nevertheless, the design of hydrogel electrolytes with desired electrochemical and mechanical properties is still challenged due to the lack of understanding of how structural features affect performances. Herein, we systematically investigate the hydrogel electrolytes for ZMAs by regulating their crosslinking and grafting structures. Experiments and theoretical simulations emphasize the importance of the network structure and the polymetric anions bonded on the hydrogel. The PSX gel crosslinked by carboxyl-grafted polyvinyl alcohol and xanthan gum shows superior performance, contributed by its abundant -COO⁻ groups and stable three-dimensional structure. The PSX electrolyte shows high ionic conductivity (18.86 mS cm⁻¹) and a considerable Zn²⁺ transference number (0.8). Zn//Zn cells with PSX electrolytes deliver long cycle lives accompanied by uniform zinc deposition, few by-products, and suppressed hydrogen evolution. When paired with V₂O₅ or active carbon cathodes, the PSX electrolyte also shows good compatibility and excellent performance. Flexible pouch cells are further demonstrated to work normally under different deformation and stress conditions.

^{Zn 2+}的不均匀通量和强溶剂化水性电解质中的离子会给锌金属阳极 (ZMA) 带来不希望的树枝状沉积和副反应。水凝胶电解质具有相当大的机械强度和有限的含水量，可以抑制枝晶生长并减轻副反应。然而，由于缺乏对结构特征如何影响性能的理解，具有所需电化学和机械性能的水凝胶电解质的设计仍然面临挑战。在此，我们通过调节其交联和接枝结构系统地研究了用于 ZMA 的水凝胶电解质。实验和理论模拟强调了网络结构和键合在水凝胶上的聚合阴离子的重要性。羧基接枝聚乙烯醇与黄原胶交联的PSX凝胶表现出优越的性能，⁻组和稳定的三维结构。PSX 电解质显示出高离子电导率（18.86 mS cm ^-1）和相当大的 Zn ²⁺迁移数（0.8）。采用 PSX 电解质的 Zn//Zn 电池可提供较长的循环寿命，同时锌沉积均匀、副产物少，并能抑制析氢。_{当与 V 2} O ₅或活性炭正极配对时，PSX 电解质也表现出良好的相容性和优异的性能。进一步证明柔性软包电池在不同的变形和应力条件下正常工作。