Disclosed herein are systems and methods in which ion-selective separation and multi-stage osmotic separation is used to produce multivalent-ion-rich process streams. According to certain embodiments, multiple separations may be used to process an aqueous feed stream containing solubilized monovalent ions and solubilized multivalent ions to produce a stream enriched in the multivalent ions. The separations may be arranged, according to certain embodiments, to enhance the overall separation process such that the product stream contains—relative to the initial aqueous feed stream—a high amount of multivalent ions, a high amount of water from the aqueous feed stream, and/or a high ratio of multivalent ions to monovalent ions.