The increasing presence of pharmaceutical active compounds (PhACs) in the environment has become a significant ecological and health concern, necessitating the development of efficient and cost-effective removal strategies. This study presents a novel composite, MIL-53(Al)@TA-Fe(Ⅲ) MPNs, integrating metal-phenolic networks (MPNs) with metal–organic frameworks (MOFs) for efficient tetracycline removal from aqueous solutions. The composite was synthesized through an environmentally benign process, involving surface modification of MIL-53(Al) with tannic acid (TA) and Fe(Ⅲ). Comprehensive characterization revealed that the optimal composite, achieved at a MIL-53(Al) to TA mass ratio of 1:1.2 and a TA to Fe(Ⅲ) molar ratio of 1:5, exhibited a large specific surface area and pore volume, contributing to its high adsorption capacity of 532 mg/g for tetracycline. Adsorption isotherm, kinetics, and thermodynamic analyses indicated that the process was spontaneous, endothermic, and chemically driven. Mechanistic studies highlighted the roles of electrostatic and π-π interactions between the composite and tetracycline molecules. The composite also demonstrated excellent reusability, retaining over 92 % of its initial adsorption capacity after five cycles. This work not only provides a green and efficient strategy for tetracycline remediation but also offers valuable insights for the development of advanced adsorbents using MPNs-modified MOFs, holding significant potential for broader environmental applications in the future.