The　functionalization　of　metal–organic　frameworks　(MOFs)　is　imperative　and　challenging　for　the　development　of　practical　MOF-based　materials.　Herein,　a　magnetically　functionalized　Zr-MOF　(Fe3O4@MOF-525)　was　synthesized　via　secondary-growth　approach　to　obtain　an　easily-separated　and　recyclable　adsorbent　for　the　removal　of　pharmaceuticals　(tetracycline　(TC)　and　diclofenac　sodium　(DF)).　After　loading　Fe3O4　nanoparticles　(NPs),　due　to　the　increase　of　micropore　volume　and　specific　surface　area　caused　by　defects,　the　adsorption　performance　of　Fe3O4@MOF-525　was　improved.　The　kinetics　could　be　described　by　the　pseudo-second-order　kinetic　model.　The　different　adsorption　capacity　and　initial　rate　were　attributed　to　the　properties　of　the　pharmaceuticals,　including　the　molecular　size　and　hydrophobicity/hydrophilicity.　In　isotherm　experiments,　the　maximum　adsorption　capacities　of　DF　and　TC　on　Fe3O4@MOF-525　calculated　by　Sips　model　reached　745　and　277　mg·g−1,　respectively.　The　thermodynamic　studies　indicated　the　adsorption　was　endothermic　and　spontaneous.　The　effect　of　pH　suggested　that　electrostatic　interaction,　π-π　interaction,　anion-π　interaction,　and　H-bonding　were　possibly　involved　in　the　adsorption　process.　The　adsorbent　was　separated　by　magnetic　and　regenerated.　Washed　with　ethanol,　Fe3O4@MOF-525　remained　about　80%　adsorption　capacity　after　four　cycles.　In-situ　photo-regeneration　under　visible-light　irradiation　was　another　attractive　method,　where　>　95%　TC　was　degraded　in　4　h.　The　reaction　with　scavengers　revealed　that　1O2　was　the　dominant　reactive　species　in　our　system,　indicating　the　occurrence　of　Type　II　photosensitization.　The　separability,　excellent　adsorption　performance,　and　recyclability　of　Fe3O4@MOF-525　may　lead　to　its　beneficial　applications　in　water　treatment.　©　2022　Elsevier　Inc.