Researchers have developed an innovative zinc-iodine (Zn-I₂) battery using molybdenum carbide (MoC) nanoclusters embedded in porous nitrogen-doped carbon fibers, integrated with atomic Zn-N4 sites. This novel design addresses key challenges associated with iodine, particularly its low electrical conductivity and the detrimental formation of soluble polyiodides that degrade capacity and corrode zinc anodes. The newly engineered Zn-SA-MoC/NCFs structure enhances electron and ion transfer and effectively confines iodine species, leading to improved redox conversion without the polyiodide shuttle effect. The Zn-I₂ battery demonstrated an impressive specific capacity of 230.6 mAh g⁻¹ at a current density of 0.5 C and exhibited 90% capacity retention after 20,000 cycles, highlighting both durability and performance. This study is groundbreaking in demonstrating the manipulation of electrocatalytic activity through the incorporation of Zn-N4 sites in MoC clusters, paving the way for high-performing iodine catalysts. The research underscores the potential of aqueous zinc-ion batteries (ZIBs) due to their environmental compatibility and the abundant availability of iodine, making them a promising candidate for future energy storage solutions. The findings contribute significant insight into advanced electrocatalysis and electronic structure modulation for improved battery performance.