In this study, MIL-101(Fe) is prepared via a facile solvent-thermal method, and then applied as catalyst for activating PMS, thus generating reactive radicals for organic dyes removal in aqueous solution. Rhodamine B (RhB), Malachite Green (MG) and Methylene Blue (MB) were selected as model pollutants. The experiments showed that MIL-101(Fe)/PMS had higher removal efficiency for dyes than MIL-101(Fe), indicating that MIL-101(Fe) can be simultaneously used as adsorbent and PMS-activating catalyst for dyes removal. The effects of initial pH and the coexisted negative ions on MB degradation were further discussed, showing that MIL-101(Fe) can degrade MB with excellent stability. Furthermore, the reactive species in MIL-101(Fe)/PMS system were deduced as sulfate radicals and hydroxyl radicals. Finally, the degradation intermediates and possible degradation pathway were investigated by LC-MS. (c) 2021 Published by Elsevier Inc.