The study presents a novel approach to enhance the performance of silver (Ag) as an anode material for capacitive deionization (CDI). Traditional Ag electrodes suffer from significant volume changes and agglomeration issues, which affect their cycling stability and efficiency. To address these challenges, the researchers developed an organic linker confinement strategy using metal-organic frameworks (MOFs). This method involves coordinating Ag nodes with organic ligands to form a well-dispersed Ag-based MOF, which enhances the utilization of active sites and interfacial stability. The resulting Ag-MOF electrode exhibits excellent Cl⁻ removal capacity (121.52 mg g⁻¹ at 20 mA g⁻¹ in 500 mg L⁻¹ NaCl solution) and a high Ag utilization rate (60.54%). After 100 cycles, it retains 96.93% of its capacity. The Cl⁻ capture mechanism of the Ag-MOF is elucidated through density functional theory (DFT) calculations, ex situ XRD, Raman, and XPS analyses. This innovative design offers valuable insights for developing high-performance conversion electrodes for CDI applications.The study presents a novel approach to enhance the performance of silver (Ag) as an anode material for capacitive deionization (CDI). Traditional Ag electrodes suffer from significant volume changes and agglomeration issues, which affect their cycling stability and efficiency. To address these challenges, the researchers developed an organic linker confinement strategy using metal-organic frameworks (MOFs). This method involves coordinating Ag nodes with organic ligands to form a well-dispersed Ag-based MOF, which enhances the utilization of active sites and interfacial stability. The resulting Ag-MOF electrode exhibits excellent Cl⁻ removal capacity (121.52 mg g⁻¹ at 20 mA g⁻¹ in 500 mg L⁻¹ NaCl solution) and a high Ag utilization rate (60.54%). After 100 cycles, it retains 96.93% of its capacity. The Cl⁻ capture mechanism of the Ag-MOF is elucidated through density functional theory (DFT) calculations, ex situ XRD, Raman, and XPS analyses. This innovative design offers valuable insights for developing high-performance conversion electrodes for CDI applications.