One-step size-controlled synthesis of ZnSe quantum dots is studied and the obtained QDs are luminescent with the emission wavelength varying over a wide range (up to 100 nm) depending on the particle size; the single-molecular precursor is an air-stable bis(phenylselenolato)zinc N,N,N′,N′-tetramethylethylenediamine (TMEDA) complex, which effectively affords different sizes of ZnSe QDs depending on growth temperatures.