Under γ-irradiation, thiacetamide (TAA) releases S2− in acidic solutions (e.g., pH = 3), and the S2− can react with available Cd2+ in soft templates to form CdS nanorods. Single-crystalline CdS nanorods were prepared in this study. The effects of various synthesis parameters on the crystalline type, morphology, average particle size, and photoelectric properties were thoroughly investigated, including the concentrations of reactants, dose of irradiation, and the type and dosage of templates. The structure and selected physical and chemical properties of products were characterized by x-ray diffraction (XRD), Fourier transform infrared (FTIR), ultraviolet-visible (UV-vis), selected area electron diffraction (SAED), transmission electron microscopy (TEM), and photoluminescence (PL) spectrophotometer techniques. Results indicated that the ratio of reactants to templates greatly affected the morphology of CdS nanorods; the types of soft templates also had significant effects on the morphology and crystalline type of the nanorod products.