Atomically precise metal nanoclusters (NCs), protected by a monolayer of ligands, are regarded as potential building blocks for advanced technologies. They are considered as intermediates between the atomic/molecular regime and the bulk. Incorporation of foreign metals in NCs enhances several of their properties such as catalytic activity, luminescence, and so on; hence, it is of high importance for tuning their properties and broadening the scope of applications. In most of the cases, enhancement in specific properties was observed upon alloying due to the synergistic effect. In the past several years, many alloy clusters have been synthesized, which show a tremendous change in the properties than their monometallic analogs. However, controlling the synthesis and tuning the structures of alloy NCs with atomic precision are major challenges. Various synthetic methodologies have been developed so far for the controlled synthesis of alloy NCs. In this perspective, we have highlighted those diverse synthetic routes to prepare alloys, which include co-reduction, galvanic reduction, antigalvanic reduction, metal deposition, ligand exchange, intercluster reaction, and reaction of NCs with bulk metals. Advancement in synthetic procedures will help in the preparation of alloy NCs with the desired structure and composition. Future perceptions concerning the progress of alloy nanocluster science are also provided. © 2021 ACS. All rights reserved.