The synthesis of monodisperse chalcopyrite (tetragonal) CuInSe2 nanocrystals is reported. The nanocrystals have trigonal pyramidal shape, and they exhibited a common crystallographic orientation when drop-cast onto carbon substrates. A crystallographic model for the nanocrystals was developed. The nanocrystals are bounded by one polar {112} surface facet and three nonpolar {114} surface facets.