The inspection of the quality of welds in battery packs plays an important role in ensuring safety during the manufacturing and operation of energy-storage devices in automotive vehicles during service. This research investigated the novel application of laser Doppler vibrometry, a widely used non-destructive optical technique for modal analysis, to the post-weld evaluation of micro-TIG-welded interconnections in lithium-ion supercells. The experimental modal analysis showed features in the modal models of the supercells that were unique to their welding conditions. The comparisons between the supercells showed an absence of linear correlations between the modal parameters and the welding current, as well as differences in the welding parameters obtained from the negative and positive terminals of the cylindrical cells. These findings suggested that the modal parameters of the supercells were more strongly influenced by the rigidity of the structural materials than by the localized compliance of the welded interconnections. While this investigation demonstrated a method for using laser Doppler vibrometry to distinguish between different welding conditions in lithium-ion supercells at a structural level, further development is needed to identify the weld quality of individual interconnections.