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Electrocatalytic nitrogen reduction (eNRR) offers a green pathway for NH3 production from N2 and H2O under ambient conditions. Transition metal oxynitrides (TMOxNy) are among the most promising catalysts but face challenges in achieving high yield and faradaic efficiency (FE). This work develops a hybrid WOxNy/WO3 catalyst with a unique heterogeneous interfacial complexion (HIC) structure. This design enables in situ generation and delivery of highly active hydrogen atoms (H*) in acidic electrolytes, promoting nitrogen hydrogenation and formation of nitrogen vacancies (Nv) on the WOxNy surface. This significantly enhances the selectivity of eNRR for NH3 synthesis while suppressing hydrogen evolution reaction (HER). A simple two-step fabrication process—microwave hydrothermal growth followed by plasma-assisted surface nitridation—was developed to fabricate the designed catalyst electrode, achieving an NH3 yield of 3.2 × 10-10 mol·cm-2·s-1 with 40.1% FE, outperforming most TMN/TMOxNy electrocatalysts. Multiple control experiments confirm that the eNRR follows a HIC-enhanced Mars-van Krevelen (MvK) mechanism.