We report a highly versatile and one-pot microwave route to the mass production of three-dimensional graphene-carbon nanotube-iron oxide nanostructures for the efficient removal of arsenic from contaminated water. The unique three-dimensional nanostructure shows that carbon nanotubes are vertically standing on graphene sheets and iron oxide nanoparticles are decorated on both the graphene and the carbon nanotubes. The material with iron oxide nanoparticles shows excellent absorption for arsenic removal from contaminated water, due to its high surface-to-volume ratio and open pore network of the graphene-carbon nanotube-iron oxide three-dimensional nanostructures.