Abstract Abstract In this work, we have proposed a concept for the generation of three-dimensional (3D) nanostructured metal alloys of immiscible materials induced by megahertz-frequency ultrafast laser pulses. A mixture of two microparticle materials (aluminum and nickel oxide) and nickel oxide microparticles coated onto an aluminum foil have been used in this study. After laser irradiation, three different types of nanostructure composites have been observed: aluminum embedded in nickel nuclei, agglomerated chain of aluminum and nickel nanoparticles, and finally, aluminum nanoparticles grown on nickel microparticles. In comparison with current nanofabrication methods which are used only for one-dimensional nanofabrication, this technique enables us to fabricate 3D nanostructured metal alloys of two or more nanoparticle materials with varied composite concentrations under various predetermined conditions. This technique can lead to promising solutions for the fabrication of 3D nanostructured metal alloys in applications such as fuel-cell energy generation and development of custom-designed, functionally graded biomaterials and biocomposites.