Coinage metal nanoclusters (MNCs) are a new type of ultra-small nanoparticles on the sub-nanometer (typically < three nm) scale intermediate between atoms and plasmonic nanoparticles. At the same time, the ultra-small size and discrete energy levels of MNCs enable them to exhibit molecular-like energy gaps, and the total structure involving the metal core and surface ligand together leads to their unique properties. As a novel environmentally friendly chromophore, MNCs are promising candidates for the construction of electroluminescent light-emitting diodes (LEDs). However, a systematic summary is urgently needed to correlate the properties of MNCs with their influences on electroluminescent LED applications, describe the synthetic strategies of highly luminescent MNCs for LEDs’ construction, and discuss the general influencing factors of MNC-based electroluminescent LEDs. In this review, we first discuss relevant photoemissions of MNCs that may have major influences on the performance of MNC-based electroluminescent LEDs, and then demonstrate the main synthetic strategies of highly luminescent MNCs. To this end, we illustrate the recent development of electroluminescent LEDs based on MNCs and present our perspectives on the opportunities and challenges, which may shed light on the design of MNC-based electroluminescent LEDs in the near future.