M. aeruginosa removal by Fe2+/persulfate process is feasible. M. aeruginosa removal rate depended on the ratio of [Fe2+]:[S2O82−] and S2O82− dosage. M. aeruginosa removal was associated with oxidative damage by SO4−. SO4− disrupted cellular structure and degraded cell inclusions of M. aeruginosa. SO4− inhibited the photosynthesis of M. aeruginosa.