This study innovated constructed an activated carbon-loaded nano-zero-valent iron (nZVI-C) enhanced membrane aerated biofilm reactor (MABR) coupled partial nitritation/anammox (PN/A) system for optimizing nitrogen and antibiotics removal. Results showed that nitrogen and antibiotic removal efficiencies of 88.45 ± 0.14% and 89.90 ± 3.07% were obtained by nZVI-C, respectively. nZVI-C hastened Nitrosomonas enrichment (relative abundance raised from 2.85% to 12.28%) by increasing tryptophan content in EPS. Furthermore, nZVI-C proliferated amo gene by 3.92 times and directly generated electrons, stimulating Ammonia monooxygenase (AMO) co-metabolism activity. Concurrently, via antibiotic resistance genes (ARGs) horizontal transfer, Nitrosomonas synergized with Arenimonas and Comamonadaceae for efficient antibiotic removal. Moreover, nZVI-C mitigated antibiotics inhibition of electron transfer by proliferating genes for PN and anammox electron production (hao, hdh) and utilization (amo, hzs, nir). That facilitated electron transfer and synergistic substrate conversion between ammonia oxidizing bacteria (AOB) and anaerobic ammonia oxidizing bacteria (AnAOB). Finally, the high nitrogen removal efficiency of the MABR-PN/A system was achieved. Display omitted •Nitrogen and antibiotic removal efficiencies of 88.45% and 89% were finally achieved.•nZVI-C enhanced tryptophan content to promote Nitrosomonas enrichment in biofilm.•nZVI-C stimulated AMO activity and enhanced Nitrosomonas co-metabolism ability.•Antibiotic removal relied on AMO and antibiotic resistance genes horizontal transfer.•Proliferation of electron transfer genes improved nitrogen removal efficiencye