A coupling process between Electrocoagulation (EC) and GAC was employed to separate dyes from aqueous solutions. The removal of an indigoid dye, namely C.I. Acid Blue 74, was tested. A novel approach for optimizing EC-based techniques is presented. In addition to maximizing removal efficiency, minimizing consumptions of energy and electrode materials were also targeted by means of multi-objective optimization in order to reduce the specific costs. A very good cost-efficiency feature of EC/GAC coupling process operated under optimal conditions to treat wastewater from dyestuff has been revealed. The independent variables considered were the current density, influent pH, contact time, granular activated carbon dose, and initial dye concentration. Simple maximization of color removal efficiency and multi-objective optimization were compared. Two different constraints were considered for each type of optimization. The determined costs outline the cheapness feature of the EC/GAC system as a potential dye wastewater treatment technology.