The ability to recover uranium from water is significant because of its potential applications on nuclear fuel capture and mitigation of nuclear wastes. In this work, a unique nanostructure is presented by which trace level (2.32-882.68 mu g/L) uranium can be quickly separated from water and encapsulated at the center of zero-valent iron nanoparticles. Over 90% of the uranium is recovered with 1 g/L nanoparticles in less than 2 min. Near atomic-resolution elemental mapping on the U(VI) intraparticle reactions in a single iron nanoparticle is obtained with aberration corrected scanning transmission electron microscopy, which provides direct evidence on U(VI) diffusion, reduction to U(IV), and deposition in the core area.