Phase control has been achieved in the synthesis of magnetic iron sulfide nanocrystals by the use of a single source precursor, a cubane type Fe-S cluster, bis(tetra-n-butylammonium) tetrakis[benezenethiolato-μ3-sulfido- iron]. This cluster cleanly decomposes in alkylamines to yield nanocrystals whose composition, structure, and dimensions are dependent on the temperature employed. At low temperatures, pyrrhotite type Fe7S8 nanocrystals with an average diameter of 5.6 nm are obtained. Higher temperatures yield griegite-Fe3S4 nanocrystals whose dimensions are tunable in the range 2.5-4.5 nm. All the obtained nanocrystals are superparamagnetic at room temperature. Copyright © 2008 American Chemical Society.