Optoelectronic cluster materials emerge rapidly in recent years especially for light-emitting devices, owing to their 100 % exciton harvesting and unique organic-inorganic hybrid structures with tunable excited-state characteristics for thermally activated delayed fluorescence and/or phosphorescence and inheritable photo- and thermo-stability. However, for efficient electroluminescence, excited-state compositions of cluster emitters should be tuned through ligand engineering to enhance ligand-centered radiative components and reduce cluster-centered quenching states. Nonetheless, the balance of optoelectronic properties requires delicate and controllable ligand functionalization. On the other hand, in addition to balancing carrier fluxes, it showed that device engineering, especially host matrixes and interfacial optimization, can not only alleviate triplet quenching, but also modify processing and passivate defects. As consequence, the record external quantum efficiencies of cluster light-emitting diodes already reached ≈30 %. Herein, we overview recent progress of electroluminescent cluster materials and discuss their structure-property relationships, which would inspire the continuous efforts making cluster light-emitting diodes competent as the new generation of displays and lighting sources.