In this perspective, we provide an overview of the recent achievements in luminescent lanthanide-based molecular cluster-aggregates (MCAs) and illustrate why MCAs can be seen as the next generation of highly efficient optical materials. MCAs are high nuclearity compounds composed of rigid multinuclear metal cores encapsulated by organic ligands. The combination of high nuclearity and molecular structure makes MCAs an ideal class of compounds that can unify the properties of traditional nanoparticles and small molecules. By bridging the gap between both domains, MCAs intrinsically retain unique features with tremendous impacts on their optical properties. Although homometallic luminescent MCAs have been extensively studied since the late 1990s, it was only recently that heterometallic luminescent MCAs were pioneered as tunable luminescent materials. These heterometallic systems have shown tremendous impacts in areas such as anti-counterfeiting materials, luminescent thermometry, and molecular upconversion, thus representing a new generation of lanthanide-based optical materials.