One-step purification and desalination The purification of water for drinking purposes can require multiple filtration steps and technologies to remove contaminants such as salts and heavy metals. Some contaminants could have value if recovered, but these are often discharged in the waste streams. Uliana et al. describe a general approach for the fabrication of robust, tunable, adsorptive membranes through the incorporation of porous aromatic framework (PAF) nanoparticles into ion exchange membranes such as those made from sulfonated polymers. Salts are removed using a series of cation and anion exchange membranes, and the PAF particles can be selected to capture specific target ions, such as those of copper, mercury, or iron. This allows for simultaneous desalination and decontamination of the water. Science, this issue p. 296 Technologies that can efficiently purify nontraditional water sources are needed to meet rising global demand for clean water. Water treatment plants typically require a series of costly separation units to achieve desalination and the removal of toxic trace contaminants such as heavy metals and boron. We report a series of robust, selective, and tunable adsorptive membranes that feature porous aromatic framework nanoparticles embedded within ion exchange polymers and demonstrate their use in an efficient, one-step separation strategy termed ion-capture electrodialysis. This process uses electrodialysis configurations with adsorptive membranes to simultaneously desalinate complex water sources and capture diverse target solutes with negligible capture of competing ions. Our methods are applicable to the development of efficient and selective multifunctional separations that use adsorptive membranes. High-performance adsorptive membranes enable one-step desalination of complex water sources and target solute capture. High-performance adsorptive membranes enable one-step desalination of complex water sources and target solute capture.