One-dimensional zinc-blende CdTe nanocrystals were successfully synthesized by a green and ambient pressure aqueous solution synthesis at relatively low temperature. The synthesized nanocrystallites were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), high-resolution TEM (HRTEM), and energy-dispersive X-ray spectroscopy (EDX), and chemical reactions of the aqueous medium synthesis were described. The resultant morphology of ZB-CdTe nanocrystals derived from different reaction solutions showed that the initial tellurium precursor concentration was a crucial factor determining the shape-controllable growth. The degradation of Te monomer concentration in reaction solutions with synthesis temperature and time were experimentally monitored, indicating that about 70−80% consumption of active Te monomer concentration was completed in temperature rise range within early 15 min. This implied that there was a burst of homogeneous nucleation and spherical growth in this period of ti...