The optical and vibrational properties of Pt- and Ni-centered Pb-Zintl-ion clusters have been investigated by UV/Vis and FTIR spectroscopy. Computational studies have been performed to better interpret the experimental data, due to a lack of any FTIR and UV/Vis spectroscopic studies on these clusters or similar ones in the literature. UV/Vis spectroscopic analyses show an asymmetric broad absorption band, with a maximum at 265 nm for both Pt- and Ni-centered Pb clusters. FTIR spectroscopic analysis demonstrated that the vibrational modes of the clusters appear at the low-frequency (terahertz) range of the spectrum. Vibrational modes of [Pt@Pb12]2- and [Ni@Pb12]2- are observed at 74 cm-1, and those of [Ni@Pb10]2- appear at 86, 143, and 200 cm-1. Similarities between simulated and experimental spectra strongly support isolated cluster behavior. [Pt@Pb12]2-, [Ni@Pb12]2-, and [Ni@Pb10]2- are the only Zintl ion clusters that have been characterized with UV/Vis and FTIR spectroscopic analyses to elucidate their optical and vibrational properties. [ABSTRACT FROM AUTHOR]