Lacking electron donors generally causes poor denitrification performance in constructed wetlands (CWs). In this study, iron scraps (ISs) and elemental sulfur (S0) were employed as electron donors in different surface flow constructed wetlands (SFCWs): control (C-SF), ISs added (Fe-SF), S0 added (S-SF), and ISs and S0 combined (Fe + S-SF) to investigate the performance and mechanism of nitrogen (N) removal through continuous flow and batch experiments. The impact of hydraulic retention times (HRTs) and temperatures on N removal was explored. The combined use of ISs and S0 significantly improved nitrate (NO3− -N) removal in Fe + S-SF compared to the other SFCWs. During the 3-d HRT at 25 °C, the average NO3− -N removal efficiency in Fe + S-SF reached the highest value of 71.66 ± 12.54%, reducing NO3− -N concentrations from 12.03 mg/L to 3.47 mg/L. The results of the batch experiments revealed an N removal pattern that aligned with the findings of the continuous flow experiment. The microbial community analysis revealed a selective enrichment of key functional genera (e.g., Ferritrophicum and Dechloromonas), contributing to enhanced N removal in Fe + S-SF. These findings suggest that the synergistic use of ISs and S0 can achieve better denitrification efficiency and potentially be utilized for enhanced N removal from low C/N wastewater.