The overuse of phosphate fertilizers has caused significant environmental and economic issues, including eutrophication, soil degradation, and disruptions to global phosphorus cycles. We investigate the PEI/PMVEMA hydrogel system, which offers a solution by demonstrating high phosphorus capture and recovery performance. The system operates effectively across a broad pH range (2.0–8.0) with a maximum capture capacity of ~ 65 - 100 mg P/g sorbent, exhibiting superior selectivity for phosphate over nitrate (α ≈ 50), in a batch and under continuous flow, which is a common limitation in wastewater treatment technologies. Additionally, it achieves a high desorption efficiency of 96-99% at pH 11.0 over multiple regeneration cycles, thus enabling efficient phosphate recovery and reuse. The hydrogel system offers high capacity, selectivity, reusability, and scalability while avoiding energy-intensive procedures. Its ability to recover phosphorus as a fertilizer aligns with circular economy principles, reduces reliance on mined phosphate, addresses overall global food security, and mitigates surface water pollution by preventing runoff-induced eutrophication.