Divalent cations, especially calcium (Ca 2ϩ ), are known to significantly affect the performance of anionic surfactants and polymers used in enhanced oil recovery (EOR) processes. An efficient technique to remove Ca 2ϩ from brine is reported, which is based on selective adsorption of Ca 2ϩ onto functionalized iron oxide magnetic nanoparticles (IOMNPs). Upon adsorption, the IOMNPs can be separated by applying a magnetic field, leaving behind softened water.IOMNP was synthesized by coprecipitation, and the amine-functionalization of its surface was obtained according to an aqueous APTES coating process. Chelating agent, polyacrylic acid (PAA), was successfully coated on amine-functionalized IOMNPs via amidation of carboxylic acid using 1-ethyl-3-(3-dimethylaminopropyl) carbodiimide (EDC). PAA modification significantly enhanced the adsorption capacity of IOMNPs due to their great ability to chelate Ca 2ϩ . The effect of pH on adsorption capacity was also investigated. The adsorption capacity of Ca 2ϩ onto PAA-IOMNPs was found to be as high as 57.2 mg/g at pH 7 from the 400 mg/L Ca 2ϩ solution. However, in American Petroleum Institute (API) standard brine (8ϫ10 4 mg/L NaCl and 2ϫ10 4 mg/L CaCl 2 ), the adsorption capacity of IOMNPs decreased to 9.8 mg/g since the high salinity screens the charges on the surface of PAA-IOMNPs and results in the formation of nanoparticle aggregates. PAA-IOMNPs can be reused after treated by acetic acid solution.A geochemical model was developed to describe the competitive adsorption of Ca 2ϩ and H ϩ onto amine-functionalized IOMNPs as a function of solution pH and Ca 2ϩ concentration. Comparison between the model and the experiments shows that the adsorption isotherms predict the behavior of the system very well. Below pH 4, adsorption of Ca 2ϩ is negligible and becomes important above pH 7. This opens the possibility of recovering the nanoparticles after the divalent cation removal, and reusing them for the repeated water softening.