While the low-absorption cross section of lantha- nide-based upconversion systems, in which the trivalent lanthanides (Ln3+) are responsible for converting low- to high- energy photons, has restricted their application to intense incident light, the emergence of a cascade sensitization through an organic dye antenna capable of broadly harvesting near-infrared (NIR) light in upconversion nanoparticles opened new horizons in the field. With the aim of pushing molecular upconversion within the range of practical applications, we show herein how the incorporation of an NIR organic dye antenna into the ligand scaffold of a mononuclear erbium coordination complex boosts the upconversion brightness of the molecule to such an extent that a low-power (0.7 W·cm−2) NIR laser excitation of [L6Er(hfa)3]+ (hfa = hexafluoroacetylacetonate) at 801 nm results in a measurable visible upconverted signal in a dilute solution (5 ×10−4 M) at room temperature. Connecting the NIR dye antenna to the Er3+ activator in a single discrete molecule cures the inherent low- efficient metal-based excited-state absorption mechanism with a powerful indirect sensitization via an energy transfer upconversion, which drastically improves the molecular-based upconverted Er3+-centered visible emission.