Calcium Hardness (Ca. H) and total Hardness ions in drinkable groundwater cause great problems for the entire world especially, the population communities which are located far from surface water sources. The present study investigates the use of Sodalite Bearing Modified Illite (SBMI) as a sustainable and new technique to eliminate these ions from drinkable groundwater to compatible with the instruction of the World Health Organization. The methodology was achieved by using a new method to remove these ions’ excess calcium Hardness and total Hardness depending on two main processes; the adsorption as a first step and the coagulation-flocculation-sedimentation process as a second step. The results of this study were achieved through conducting three tasks; (1) Chemical analysis surveys for all the groundwater wells, to determine the areas which are more affected by these salts, and plot them on the location maps. (2) Conducting the alkaline modification of the Illite ore to obtain the (SBMI) which has a high surface area and high adsorption ability, and it had been characterized by using XRD, XRF, SEM, and FTIR techniques. (3) The experimental studies were conducted to evaluate the effect of the modified Illite on raw groundwater containing a high concentration of hardness ions, through the batch studies to determine the factors which affected its ability for removing these ions from groundwater. The present study illustrated that the removing efficiency for both total hardness (Ca. H + Mg. H) and calcium hardness (Ca. H) reached about 98%. Finally, the present study recommended using this technique, when there is a requirement for large quantities of treated water at a low cost.