The generation of nanoalloys of immiscible metals is still a challenge using conventional methods. However, because these materials are currently attracting much attention, alternative methods are needed. In this article, we demonstrate a simple but powerful strategy for the generation of a new metastable alloy of immiscible metals. Au_1−xNi_x 3D structures with 56 at% of nickel in gold were successfully manufactured by the pulsed laser irradiation of colloidal nanoparticles. This technology can be used for preparing different metastable alloys of immiscible metals. We hypothesise that this technique leads to the formation of alloy particles through the agglomerations of nanoparticles, very fast heating and fast cooling/solidification. Thus, we expect that our approach will be applicable to a wide range of inorganic solids, yielding even new metastable solids that fail to be stable in the bulk systems and therefore do not exist in Nature.