The maintenance of harbor waterways generates large amounts of dredged sediments which are often rich in coexisting organic and inorganic contaminants. Electrokinetic remediation treatments have recently been developed for the simultaneous removal of heavy metals and polycyclic aromatic hydrocarbons (PAHs), using various enhancing agents generally tested sequentially. In this study, different processing fluids were tested, alone or mixed, to improve the decontamination of aged model sediment contaminated with cadmium, lead, chromium, copper, zinc, and five PAHs. Nitric acid (NA) and citric acid (CA) were tested to avoid the formation of an alkaline front into the sediment and favor the metals removal, while an anionic surfactant [sodium dodecyl sulfate (SDS)] and a nonionic surfactant (Tween 20) were tested to solubilize and mobilize PAHs. Processing fluids were circulated under a constant voltage gradient of 1 V cm−1 for 10–14 days. NA showed an excellent potential to remove metals (76.8–99.9 % removal) and PAHs (70.3–89.7 % removal) in a single run. Besides, the mixture of Tween 20 and CA, more environmental friendly, could be considered as a relatively good processing fluid for the simultaneous removal of metals (10.3–90.8 % removal) and PAHs (53.6–61.6 % removal) from the fine-grained sediment, while SDS mixed to CA was not a good candidate for this purpose (0.1–65 % removal for metals and 34.1–41.0 % removal for PAHs).