Atomically precise metal nanoclusters (MNCs) represent a fascinating class of ultrasmall nanoparticles with molecule-like properties, bridging conventional metal−ligand complexes and nanocrystals. Despite their potential for various applications, synthesis challenges such as a precise understanding of varied synthetic parameters and property-driven synthesis persist, hindering their full exploitation and wider application. Incorporating smart synthesis methodologies, including a closed-loop framework of automation, data interpretation, and feedback from AI, offers promising solutions to address these challenges. In this perspective, we summarize the closed-loop smart synthesis that has been demonstrated in various nanomaterials and explore the research frontiers of smart synthesis for MNCs. Moreover, the perspectives on the inherent challenges and opportunities of smart synthesis for MNCs are discussed, aiming to provide insights and directions for future advancements in this emerging field of AI for Science, while the integration of deep learning algorithms stands to substantially enrich research in smart synthesis by offering enhanced predictive capabilities, optimization strategies, and control mechanisms, thereby extending the potential of MNC synthesis.