MIL-101-NH 2 (Fe) is one of the effective photocatalytic metal− organic frameworks (MOFs) working under visible light. However, its powder-type form inhibits reusability in practical applications. In this study, we immobilized MIL-101-NH 2 (Fe) on a polymeric microfiber mesh to improve reusability while minimizing the loss of catalytic performance. To overcome the lack of surface functionality of the nylon fibers, an atomic layer deposition Al 2 O 3 layer and NH 2 -BDC linker were introduced to facilitate uniform coating of the MOF on the fiber surface. The reactions of the metal precursor to the nylon substrate and NH 2 -BDC ligand of the MOF allow chemical bonding from the core to the shell of the entire hybrid catalytic materials. The resulting fiber-immobilized MOFs (Nylon@Al 2 O 3 @ MOF) demonstrated high photocatalytic performance in the removal of RhB and Cr(VI) as representatives of organic dyes and heavy metals, respectively, while retaining over 85% of its efficiency after five cycles.