This work focuses on the synthesis of nanocrystals with A 2 B 2 O 7 composition (in this study, A ) La, Er, or their mixture, B ) Zr, Hf, or their mixture), their structural characterization, and luminescent property measurements. It was necessary to utilize a single-source complex precursor A(OH) 3 • BO(OH) 2 • nH 2 O to synthesize these A 2 B 2 O 7 nanocrystals, by the synergistic interplay between the reduction of the transport distances of the reactive constituents to an atomic length scale and the enhanced diffusion of the reactants in the molten salt medium. This process is highly generalizable for the preparation of other complex oxide nanocrystals. Moreover, these nanocrystals possess outstanding luminescent properties, including strong photoluminescence in the infrared region, efficient pump-power dependence and excellent cathodoluminescence. These desirable properties make these nanocrystals promising for applications in display, bioanalysis, lighting, scintillating, and telecommunications.