Microbial interactions affect the biogeochemical cycles, pollutant transformation, and stable operation of constructed wetlands (CWs), and these interaction networks are vulnerable to environmental stress. Iron (Fe)-based CWs have been demonstrated as an intensified nitrogen (N) removal system, however, whether and how the addition of Fe, an exogenous environmental stressor, and its amount affect the microbial interactions and functions are poorly understood, which inevitably determine the stability and sustainability of CW system. Herein, we demonstrated that higher Fe addition could effectively improve the stability and sustainability of the CW system by regulating the diversity and interactions of the microbial communities rather than the relative abundance of functional genes. Specifically, low Fe-addition reduced the complexity and robustness of microbial network and the number of keystone taxa, while the high Fe-addition CWs showed the opposite pattern. In CWs with low Fe-addition, N-Fe cycles were accomplished by increasing competition represented by a high proportion of negative links between the same function, whereas increased cooperation was observed in CWs with high Fe-addition. Moreover, Fe addition shaped divergent N transformation processes, with denitrification-dissimilatory nitrate reduction to ammonium (DNRA) dominating in control group, and nitrification-partial denitrification/anammox (PD/A) dominating in Fe-based CWs, and the intensity of nitrification-PD/A increased with the addition amount of Fe. Our study provided insights into the potential ways to improve the stability and sustainability of Fe-CWs for intensified pollutant elimination, which would be valuable to advance the design, sustainable operation, and application of Fe-CWs.