ABSTRACT Cyanobacterial outbreaks seriously affect drinking water safety. Therefore, developing effective algal removal technologies is urgently needed. The study aims to investigate the effects of pH, electrode distance, current density, and initial algal concentration on electrochemical algae collection. Consequently, we loaded nanoscale zero-valent iron (nZVI) on activated carbon fiber/nickel foam (ACF/Ni) to form an ACF/nZVI/Ni composite cathode using the liquid phase reduction method and used titanium-based platinum plating (Pt/Ti) as the anode to construct a novel Pt/Ti- ACF/nZVI/Ni electrochemical system. The results showed that on pH of 6.0, the electrode distance was 10 mm, the current density was 75 mA/cm2, and the initial algal concentration was OD680 = 0.100; the algal cell removal rate was 94.20% after electrolysis for 30 min. This paper provides an efficient and environmentally friendly electrochemical algal removal technology for protecting the safety of drinking water and dealing with cyanobacterial outbreaks.