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In this study, the sodium perborate (SP)-activated peroxymonosulfate (PMS) process was used to enhance the coagulation efficiency of cyanobacteria with polymeric aluminum chloride (PAC), aiming to efficiently mitigate the impact of algal blooms on the safety of drinking water production. The optimal concentrations of SP, PMS, and PAC were determined by evaluating the removal rate of OD680 and zeta potential of the algae. Experimental results demonstrated that the proposed ternary PMS/SP/PAC process achieved a remarkable OD680 removal efficiency of 95.2%, significantly surpassing those obtained from individual treatments with PMS (19.5%), SP (5.2%), and PAC (42.1%), as well as combined treatments with PMS/PAC (55.7%) and PMS/SP (28%). The synergistic effect of PMS/SP/PAC led to the enhanced aggregation of cyanobacteria cells due to a substantial reduction in their zeta potential. Flow cytometry was performed to investigate cell integrity before and after treatment with PMS/SP/PAC. Disinfection by-products (DBPs) (sodium hypochlorite disinfection) of the algae-laden water subsequent to PMS/SP/PAC treatment declined by 57.1%. Moreover, microcystin-LR was completely degraded by PMS/SP/PAC. Electron paramagnetic resonance (EPR) analysis evidenced the continuous production of S O 4 • − , •OH, 1O2, and O 2 • − , contributing to both cell destruction and organic matter degradation. This study highlighted the significant potential offered by the PMS/SP/PAC process for treating algae-laden water. [ABSTRACT FROM AUTHOR]