A liquid-phase reducing method of synthesizing Pt nanocrystals was demonstrated, and dendrite-, cube-, and cuboctahedron-shaped Pt nanocrystals (NCs) with well-defined monomorphic were successfully synthesized through iodine ions mediated with the CTAB agent. When the KI concentration was increased to thirty times of K2PtCl4 at the nucleation stage, the high-quality Pt nanodendrites could be obtained. However, no matter how many KI were added at the growth age, only cube- and cuboctahedron-shaped Pt nanocrystals formed. The results of high-resolution TEM, EDX, and XRD indicated that the size and shape of Pt NCs could be turned by changing the concentration and time of KI. In the nucleation stage, it might be due to that some iodine ions adsorb on the surfaces of Pt NCs, which probably cause the rapid growth process resulting in the formation of Pt nanodendrites. In the growth stage, although high concentrations of I− ions could contribute to the shape control and generate bigger particles of Pt NCs, small Pt particles do not grow into dendrites. The insight into the role of I− ions in synthesis of Pt NCs reported here provided a viewpoint for clearly understanding the formation mechanism of anisotropic platinum nanostructures.