One of the most advantageous methods for lowering water hardness is the use of low-cost adsorbents. In this research, the effectiveness of natural zeolite (clinoptilolite type), activated carbon, and activated alumina was evaluated. These adsorbents were sequentially modified by NaCl, HCl, and NaCl-HCL to improve their ability to adsorb. The contact time and the amount of adsorbent used in the adsorption process were investigated experimentally to determine their effects. The results indicated that the best contact time for hardness reduction was 90 min, and the best concentrations of adsorbents in drinking water for zeolite, activated carbon, and activated alumina were 40, 60, and 60 g/L, respectively. In addition, for groundwater, these figures were 60, 40, and 40 g/L, respectively. The greatest possible decreases in total hardness under the best conditions by natural zeolite, activated carbon, and activated alumina adsorbents were 93.07%, 30.76%, and 56.92%, respectively, for drinking water and 59.23%, 15.67 %, and 39.72% for groundwater. According to the results obtained from experiments, NaCl-modified zeolite, natural zeolite, and NaCl-HCl-modified activated carbon performed better in terms of parameter reduction. The equilibrium data were well fitted by the Langmuir isotherm model, whereas the kinetic data for the adsorption process were consistent with the pseudo-second-order model. The equilibrium study of the adsorption process by the Morris–Weber model revealed that both chemical and physical adsorption are involved.