Metal‐organic frameworks (MOFs) had been widely used in adsorption, but nanoscale MOFs always caused secondary pollution which attributed to the difficultly of removing from water completely. To solve the problem, nanoscale metal‐organic framework MIL‐53(Fe) was uniformly grown onto carbon nanotubes (CNTs)/ethylene vinyl acetate (EVA) fiber to obtain MIL‐53(Fe)/CE fiber, and the loading content of MIL‐53(Fe) reached to 60.6 wt %. The MIL‐53(Fe)/CE fiber exhibited excellent adsorption capacity for congo red (CR) and medium orange 1 (MO1), which the removal was 99.4 % and 96.8 %. In addition, the composite could release nearly all adsorbed dyes after 1 h, which had the potential of recycling. The adsorption content of pure MIL‐53(Fe) for MO1 was about 68.4 % after 4 cycles, and the composite reached to 82.4 % after 9 cycles, implying the desirable reusability of composite. The MIL‐53(Fe)/CE fiber displayed potential application prospects in dye adsorption because of its ideal separation property, fast dye releasing and good recyclability.