A facile one-pot synthetic approach, using oleic acid and oleylamine as composite stabilizers combined with high-temperature treatment in 1-octadecene, has been developed for the preparation of monodisperse and uniform lanthanum phosphate and europium-doped lanthanum phosphate nanocrystals. In particular, with the present synthetic approach, the size of the resulting nanocrystals could be tuned precisely and continuously from 3.5 to 6.5 nm by seed-mediated epitaxial growth. The as-obtained uniform nanocrystals with hydrophobic surfaces, which show efficient photoluminescence, could be easily dispersed in nonpolar solvents. More importantly, these nanocrystals can also be easily modified to water-dispersed ones with hydrophilic surfaces for potential use in in vitro imaging in bioanalysis. In addition, a synthetic mechanism for these monodisperse nanocrystals is presented and discussed.