Gold-coated gadolinium nanocrystals, with an average diameter of 3.20 ± 0.35 nm, have been synthesized at ambient temperature by alkalide reduction. Whereas uncoated gadolinium nanoparticles react violently with air and water, the gold-coated gadolinium nanocrystals reported here show no reaction even upon long-term exposure. This is the first example of air- and water-stable lanthanide metal nanocrystals, which may allow for the development of magnetic and biomedical applications of gadolinium and other lanthanide metal and alloy nanocrystals.