<p>Tetracyclines (TCs), a class of broad-spectrum antibiotics, are major contaminants in water, have adverse effects on the ecosystem, and are toxic non-target organisms. A straightforward and efficient strategy for both the detection and removal of TCs from water remains highly desirable but is challenging to develop. In this study, a dual-functional platform for detecting and removing TCs was developed using highly stable silver-based metal-organic frameworks (Ag-MOFs). This platform enabled the specific detection of TCs over a broad concentration range (from 1 × 10⁻¹⁰ to 1 × 10⁻³&#xa0;mol/L), with a low detection limit of 8.4&#xa0;nM. By leveraging its high surface area, the Ag-MOFs exhibited exceptional adsorption capacities, reaching 276&#xa0;mg/g for chlortetracycline. To elucidate the potential response mechanism and electronic transfer pathway, density functional theory calculations and charge density difference analyses were performed. This Ag-MOFs-based platform achieved both rapid detection and efficient removal of TCs from the environment. The design principles proposed herein are expected to inspire the development of novel platforms for the simultaneous sensing and removal of specific pollutants.</p> Graphical Abstract <p></p>