Fluoride is the most electronegative element and has a strong affinity for aluminium. Owing to this fact, most of the techniques used for fluoride removal utilized aluminium compounds, which results in high concentrations of aluminium in treated water. In the present paper, a new approach is presented to meet the WHO guideline for residual aluminium concentration as 0.2 mg/L. In the present work, the electrocoagulation (EC) process was used for fluoride removal. It was found that aluminium content in water increases with an increase in the energy input. Therefore, experiments were optimized for a minimum energy input to achieve the target value (0.7 mg/L) of fluoride in resultant water. These optimized sets were used for further investigations of aluminium control. The experimental investigations revealed that use of bentonite clay as coagulant in clariflocculation brings down the aluminium concentration of water below the WHO guideline. Bentonite dose of 2 g/L was found to be the best for efficient removal of aluminium.