The morphology of CuInSe2 nanocrystals plays a key role in their functional properties. Achieving controllable morphology is significant for studying their structures and novel properties. Here, CuInSe2 nanocrystals with a trigonal-pyramidal shape have successfully been synthesized by a facile solution-phase method. The nanocrystals were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), and X-ray photoelectron spectroscopy (XPS), etc. The morphological evolution of the CuInSe2 nanocrystals was illustrated by tuning the injection temperature of oleylamine-selenium (OAm-Se). In addition, CuInSe2 nanocrystals with spherical and ellipsoidal shapes were also obtained when copper stearate was used as the copper precursor.