A new technique based on the combination of an activated alumina column and an electrochemical system for fluoride removal from water is reported in this study. In the first step, the optimization of the process was achieved under various experimental parameters (volumetric flow, temperature, pH, initial fluoride concentration and hardness) with a synthetic solution. The comparison of the performance of the current activated alumina process and the electrosorption system proved to be more efficient than the latter in removing fluoride from water. Thus, the fluoride sorption capacity at the breakthrough point of the activated alumina column reached 3.8 mg F-/L. It was increased by about 60% by means of the electrochemical process than the results obtained in current mode. Moreover, it was found that the electrosorption system could be utilized to regenerate the saturated activated alumina. In the second step, the electrosorption process was utilized to treat Sahara drinking water naturally contaminated with fluoride (3 mg/L) under optimum conditions previously determined. The electrosorption process coupled with activated alumina column has been successfully applied for fluoride removal from drinking water.