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• ZIF-8 is anchored on 2D amino-functionalized Al-MOF via the MOF-on-MOF method. • ZIF-8 significantly boosts the affinity and adsorption capability toward TCs. • Synergistic effect of pyridine N and NH 2 enhances the detection sensitivity. • Simultaneous high-performance capture and sensing of TCs from contaminated water. • Satisfied recoveries (93-105%) and RSD s (≤ 5.0%) for real applications. The increasing misgivings of environmental pollution derived from antibiotic residues make it imperative to explore a bifunctional platform for synchronous monitoring and removal of antibiotics. Herein, zeolite imidazolate framework-8 (ZIF-8) is anchored on two-dimensional (2D) amino-functionalized Al-metal organic framework (NH 2 -MIL-53(Al)) nanoplates to construct a dual metal–organic frameworks smart platform (ZIF-8/NH 2 -MIL-53(Al)) for simultaneous capture and fluorescence sensing of tetracyclines (TCs). ZIF-8 nanoparticles anchored on 2D nanoplates having a smaller size and a larger specific surface area boost the adsorption capabilities (561, 533, 526 and 578 mg g−1 for doxycycline (DOX), tetracycline (TET), oxytetracycline (OTC) and chlortetracycline (CTC), respectively). Notably, the pyridine N of ZIF-8 cooperated with the abundant NH 2 on the surface of NH 2 -MIL-53(Al) exhibits high affinity toward TCs, remarkably enhancing the sensitivity by facilitating the photo-induced electron transfer and the inner-filter effect. The LOD s (1.2 μg L−1 for TET, DOX, OTC and 2.2 μg L−1 for CTC, respectively) are at least 10-fold lower than those of NH 2 -MIL-53(Al) and are comparable or superior to those of reported sensors. The dual metal–organic frameworks smart platform presents satisfactory reliabilities and accuracies for detecting TCs in real samples, which anticipates new routes to develop integrated systems for simultaneous capture and detection of organic pollutants. [ABSTRACT FROM AUTHOR]