Chalcopyrite copper iron sulfide (CuFeS2) nanocrystals have gained recent interest due to their metal-like optical response, despite their complete lack of free charge carriers. These novel optical characteristics make CuFeS2 an intriguing material for a variety of applications, including photovoltaics and photothermal applications. Unfortunately, synthesis of high quality CuFeS2 nanoparticles is difficult due to the difference in the reactivity of the two cations, often resulting in binary or polydisperse nanocrystals. To gain better control over nanocrystal morphology, we synthesized CuFeS2 nanocrystals via a hot injection method and studied the effect of the cation precursor ratio on the resulting properties of the nanocrystals. Transmission electron microscopy, X-ray diffraction, and UV-vis-NIR spectroscopy were used to analyze the nanocrystal composition, morphology, and optical characteristics. Based on the characterization data, a 1:2 molar ratio of copper to iron precursor was optimal for producing high quality, monodisperse CuFeS2 nanocrystals. These developments in morphological control will aid in future studies of quasi-static resonances in these materials.