The present invention provides a electrolytic defluoridation process. The process is based on the principle of electrolysis using aluminium plate electrodes placed in raw water containing excess fluoride. During electrolysis, anodic aluminium forms polyhydroxy aluminium species and fluoride is removed by complex formation with these species, adsorption, coagulation and settling. In addition to fluoride removal, the process also reduces total dissolved solids which include hardness, nitrate and microbial contamination from raw water. The taste of the treated water is palatable. The process is suitable for provision of safe potable water in fluoride affected areas. The process operated in batches as per requirement for drinking and cooking purposes. It is simple to fabricate, easy to operate even by unskilled persons, and requires minimum maintenance.