A novel dual-ligand Fe-based MOFs (D-Fe-MOFs) was synthesized with dielectric barrier discharge (DBD) plasma for the first time, which exhibited efficient simulated solar light photocatalytic performance. 1,3,5-Benzenetricarboxylicacid (H3BTC) and 2-methylimidazole (2MI) were used as organic ligands for D-Fe-MOFs synthesis. Compared with S-Fe-MOFs, which used H3BTC as organic ligand, D-Fe-MOFs showed larger specific surface area and larger pore volume. The molar ratio of different organic ligands had a great influence on the photocatalytic performance of the catalyst, and H3BTC:2MI = 1:1 was the most beneficial to the photocatalytic performance. D-Fe-MOFs synthesized under the conditions of discharge voltage 15.6 kV, discharge current 1.5A and discharge time 1.5 h had higher thermal stability and showed high photocatalytic performance with degradation rate of 97% in 48 min for MO (20 mg/L) under simulated solar light. D-Fe-MOFs synthesized with DBD plasma exhibited sufficient conduction and valence band positions, which was beneficial for photocatalysis, where ·O2–, ·OH and h+played important roles.