In this study, pore‐filling anion‐exchange membranes (PFAEMs) incorporating (vinylbenzyl)trimethylammonium chloride (VBTA) and 1,3,5‐triacryloylhexahydro‐1,3,5‐triazine (TATA) were investigated to enhance the initial durability and performance of AEM water electrolysis (AEMWE). The optimized VBTA‐TATA‐20 membrane exhibited superior OH − conductivity (99.5 mS·cm −1 at 60°C) and enhanced mechanical and dimensional stability compared to the commercial PiperION membrane. Building upon these intrinsic properties, AEMWE performance was systematically optimized under varying temperatures, flow rates, and flow configurations. While the transition from symmetric to asymmetric flow (dry cathode) resulted in a slight performance trade‐off, VBTA‐TATA‐20 demonstrated remarkable adaptability to practical operating conditions. Notably, although the ex situ areal specific resistance (ASR) of VBTA‐TATA‐20 was 129.7% of PiperION, the in situ ohmic resistance ( R ohmic ) gap derived from I-V narrowed to 108.9% under dry cathode conditions. This discrepancy suggests that the VBTA‐TATA‐20 membrane may facilitate more effective water retention and ionic transport under asymmetric dry cathode operation, thereby potentially mitigating membrane drying induced by Joule heating. In 100 h initial durability tests under asymmetric flow, VBTA‐TATA‐20 maintained a stable voltage plateau without the irreversible degradation observed in PiperION, despite exhibiting reversible voltage fluctuations attributed to dynamic gas transport in the cathode. These findings suggest that the triazine‐based cross‐linked architecture may contribute to enhanced mechanical robustness and improved water management, supporting stable operation under practical asymmetric flow conditions.
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