Constructed wetlands (CWs) have been widely used to remove nitrogen in the effluent from sewage plants. Still, the removal capacity of nitrate (NO3−-N) in CWs is unsatisfactory due to the insufficient electron donor. This study explored the role of activated carbon (AC) in nitrogen removal and greenhouse gas (GHG) emissions reduction in different iron-based CWs. Long-term experimental results showed that pyrite and sponge iron-based CWs had higher NO3−-N removal rates (98.18 % and 94.10 %). Compared with the control group, AC promoted their total nitrogen (TN) removal efficiency (78.87–87.59 %) and reduced GHG emissions (CO2: 3.79–4.11 %, N2O: 2.97–8.78 %, CH4: 9.93–10.73 %). Moreover, AC not only promoted the values of electron transfer system activity (ETSA), the activity of nitrate reductase and nitrite reductase, but also significantly increased the microbial diversity and abundance of the substrate layer in pyrite/SI- based CWs. The relative abundance of the dominant bacteria in CWs with pyrite coupling with AC (PC-CW) was the highest (nirS: 77.60 %, nosZ: 88.98 %) compared with the other CWs. The higher relative abundance of Dechloromonas and Thiobacillus in PC-CW indicated that the composite substrates of pyrite and AC promoted the extracellular electron transfer of denitrifying microorganisms. This study provides new insights into optimizing inorganic electron donors to improve the removal of NO3−-N and the reduce of GHG emissions in CWs for low C/N wastewater treatment.