Structure, stability, and vibrational IR and Raman spectra of I(2)(center dot)(center dot-)nCO(2) clusters (n = 1-10) are reported based on first-principle electronic structure calculations. Several close-lying minimum energy structures are predicted for these solvated clusters following the quasi Newton-Raphson procedure of geometry optimization. Search strategy based on Monte-Carlo simulated annealing is also applied to find out the global minimum energy structures of these clusters. Successive addition of solvent CO2 molecules to the negatively charged diatomic solute, I-2(center dot-), is fairly symmetrical. Energy parameters of these solvated clusters are calculated following second-order Moller-Plesset perturbation (MP2) as well as coupled cluster theory with 6-311+G(d) set of basis function (I atom is treated with 6-311G(d) set of basis function). The excess electron in these solvated clusters is observed to be localized mainly over the two I atoms. Average interaction energy between the anionic solute, I-2(center dot-), and a solvent CO2 molecule is similar to 129 meV in I(2)(center dot)(center dot-)nCO(2) clusters, and the average interaction energy between two solvent CO2 molecules is similar to 85 meV in the case of neutral (CO2)(n) clusters at MP2 level of theory. IR spectra show similar features in all these solvated clusters, depicting a strong band at similar to 2330 cm(-1) for C-O stretching and a weak band at similar to 650 cm(-1) for CO2 bending modes. Degeneracy of the bending mode of a free solvent CO2 unit gets lifted when it interacts with the charged Solute I-2(center dot-) to form a molecular cluster because of the change in structure of solvent CO2 units. The vibrational band at the bending region of CO2 in the Raman spectra of these anionic clusters shows a characteristic feature for the formation of I-2 center dot-(center dot)nCO(2) clusters showing a Raman band at similar to 650 cm(-1).