Electrokinetic remediation, effective for low-permeability sediments, can simultaneously remove both organic and inorganic contaminants. This study investigated its application to dredged sediments from Camorim Lagoon (Jacarepaguá lagoon complex, Rio de Janeiro), known to be contaminated with potentially toxic metals (chromium, copper, lead, zinc, and nickel). A buffer solution-controlled pH changes, while the complexing agent ethylenediaminetetraacetic acid (EDTA) and humic substances facilitated metal desorption and removal. Treatments utilizing EDTA (EK2 and EK3) achieved lower final concentrations of zinc and lead. Notably, EK1 (freshwater only) achieved the lowest nickel concentration observed in the anodic section. EK1 also achieved the lowest copper concentration; however, none of the treatments reached regulatory limits for copper. Chromium, being the least mobile metal, accumulated in the middle section for all treatments. Electrokinetic remediation demonstrated significant variability in the effectiveness of the evaluated electrolytes, depending on the specific contaminant element present in the dredged sediments.