Holistic understanding of electrocatalytic behaviors and microbiological mechanisms respond to voltage level (VL) benefits constructing performance-pathway-community linkages in iron anode-assisted constructed wetlands (IACWs). Herein, five solar-driven IACWs at 0, 1, 5, 10, and 15 V were established to treat secondary effluent for 109 days across moderate to low water temperatures (WTs). Results showed that total nitrogen (TN) (4.87-54.42%) and total phosphorus (TP) (20.66-97.35%) removals both ascended as VL raised, which primarily occurred in the cathodic regions and anodic upstream, respectively. More sustainable nitrogen elimination was achieved at lower VLs (≤ 5 V). Electrochemical contribution quantification revealed that electrochemical denitrogenation strengthened as VL improved (144.3-965.7 mg m