Ammonium in domestic wastewater represents both an environmental challenge and a valuable resource capable of supplying up to 30% of global nitrogen fertilizer demand, but traditional treatment methods focus on energy-intensive removal rather than recovery. While electrochemical technologies offer a promising alternative, they are currently limited by low ion-storage capacities or excessive energy inputs. To achieve selective and sustainable ammonium recovery, this project introduces a collaborative, interdisciplinary approach that synergistically leverages PI Kim’s expertise in electrochemical separation and Co-PI Zhou’s expertise in advanced membrane fabrication to develop novel defect-sealed membranes decorated with ammonium-selective Prussian blue analogues (PBAs). By utilizing the unique cubic framework of PBAs, the team will promote preferential transport of ammonium over competing ions through a PBA-decorated membrane under an electric field. Simultaneously, to overcome the membrane defects identified in the PI’s prior layer-by-layer membrane assemblies, the Co-PI will employ a counter-diffusion interfacial polymerization strategy to form localized polyamide plugs within interparticle non-selective voids, blocking leakage without compromising the active PBA surface. Ultimately, this coordinated effort provides a transformative, scalable platform for wastewater remediation and nutrient recovery, directly advancing the goals of resource sustainability and a circular economy.