The optical absorption, emission, FT Raman, one-photon excitation, two-photon excitation, and luminescence lifetime measurements are reported for UO2Cl42- in 40:60 AlCl3-EMIC (where EMIC equivalent to 1-ethyl-3-methylimidazolium chloride), a room-temperature ionic liquid. Comparison of the spectra with previous results from single crystals containing UO2Cl42- allowed the characterization of four ground-state vibrational frequencies, two excited-state vibrational frequencies, and the location of eight electronic excited-state energy levels. The vibrational frequencies and electronic energy levels are found to be consistent with the UO2Cl42- ion. Comparison of the one-photon and two-photon excitation spectra, and the relative intensities of the transitions in the emission spectrum indicate that the center of symmetry is perturbed by an interaction with the solvent.