Electrocoagulation (EC) was studied in this study as a potential alternative approach for treating Olive Mill Wastewater (OMW). Aluminum plates were utilized as anode and cathode to evaluate the removal of Chemical Oxygen Demand (COD) from OMW and the aluminum electrode’s weight loss. Central Composite Experimental Design (CCD) and Response Surface Methodology were used to optimize its performance. Anodes were weighed before and after each electrocoagulation experiment, to compare the experimental and the theoretical dissolved aluminum weights calculated using Faraday’s law. We discovered the following EC conditions for CCD: current density = 15 mA/cm2, pH = 4, and electrolysis time of 30 min. Under these conditions, the maximum COD removal ratio was 41%, equating to an Al weight loss of 288.89 g/m3 at an estimated operating cost of 1.60 USD/m3. According to the response optimizer, the most economical operating settings for COD removal efficiency of 58.888% are pH 4, a current density of 18.41 mA/cm2, electrolysis time of 36.82 min, and Al weight loss of 337.33 g/m3, with a projected running cost of 2.00 USD/m3.