<p>Aqueous zinc-ion batteries (AZIBs) are safe and cost-effective, making them ideal for large-scale energy storage and wearable electronics. Nevertheless, the advancement of AZIB technology faces constraints due to limited energy storage capability and degraded cyclability, primarily attributed to the absence of optimal cathode materials. In this study, two structurally similar but chemically different covalent organic framework materials (Aza-COF-1L and Aza-COF-2) were synthesized. Notably, Aza-COF-1L is easier to synthesize and features abundant pyrazine redox-active sites, a well-defined porous structure, and intrinsic stability. Consequently, Aza-COF-1L exhibited an electrochemical performance superior to that of Aza-COF-2. Aza-COF-1L achieved initial capacities of 368.58, 345.96, and 327.82 mAh·g⁻¹ at 0.1, 0.5, and 1 A·g⁻¹, respectively. After 800 cycles at 1 A·g⁻¹, Aza-COF-1L maintains a specific capacity of 136.38 mAh·g⁻¹. In contrast, Aza-COF-2 exhibited an initial capacity of 117.79 mAh·g⁻¹ at 0.1 A·g⁻¹, and its capacity significantly decreased during cycling. Additionally, the contribution of the C=N pyrazine redox site in Aza-COF-1L to battery capacity during charging and discharging was experimentally analyzed. These results provide valuable guidance for the development of high-performance organic cathode materials for use in AZIBs.</p>