A three-component composite, Fe3O4@C@layered double hydroxide (Fe3O4@C@Ni-Al LDH), was prepared through a two-step layer-by-layer route. The carbon-coated Fe3O4 nanoparticles (Fe3O4@C) were first synthesized by a hydrothermal reaction, and then Ni-Al LDH nanosheets were anchored onto Fe3O4@C via an in situ growth method. The as-obtained Fe3O4@C@Ni-Al LDH magnetic composite was applied as magnetic adsorbent for the extraction of uranium(VI) ions from aqueous solutions. The maximum adsorption capacity of the composite for uranium(VI) ion was 174.1 +/- 0.2 mg g(-1), showing a high efficiency for the removal of uranium(VI) from aqueous solution. In addition, the composite can be easily separated from the solution by a magnet after the adsorption process. The results indicate that Fe3O4@C@Ni-Al LDH composite can be used as a potential adsorbent for sorption uranium(VI) and also provide a simple, fast separation method for removal of uranium(VI) ions from aqueous solution.