The productivity of the capacitive deionization (CDI) system is enhanced by determining the optimum operational and structural parameters using radial movement optimization (RMO) algorithm. Six different parameters, i.e., pool water concentration, freshwater recovery, salt ion adsorption, lowest concentration point, volumetric (based on the volume of deionized water), and gravimetric (based on salt removed) energy consumptions are used to evaluate the performance of the CDI process. During the optimization process, the decision variables are represented by the applied voltage, capacitance, flow rate, spacer volume, and cell volume. Two different optimization techniques are considered: single-objective and multi-objective functions. The obtained results by RMO optimizer are compared with those obtained using a genetic algorithm (GA). The results demonstrated that the RMO optimization technique is useful in exploring all possibilities and finding the optimum conditions for operating the CDI unit in a faster and accurate method.