To develop the next generation of hypergolic, ionic-liquid-based fuels, it is important to understand the fundamental reaction mechanisms for the oxidation of ionic liquids (ILs). We consequently studied the oxidation of a levitated 1-butyl-3-methylimidazolium dicyanoborate ([BMIM][DCBH]) droplet by nitrogen dioxide (NO2). The properties of [BMIM][DCBH], including short ignition-delay times, low viscosities, and a wide liquid temperature range, make the ionic liquid especially suitable as a component of a hypergolic fuel. The chemical modifications were monitored with Fourier-transform infrared (FTIR), Raman, and ultraviolet-visible spectroscopies. To identify changes induced by the oxidation, it was first necessary to assign vibrational modes to the FTIR and Raman spectra of unreacted [BMIM] [DCBH]. The new features in the oxidized FTIR and Raman spectra could then be identified and assigned on the basis of the possible functional groups likely to form through addition with a nitrogen and an oxygen atom of nitrogen dioxide creating a new bond with the ionic liquid. The assignments suggest that organic nitro-compounds and boron-nitrogen and boron-oxygen containing compounds were produced. A large decrease in the intensity of some [DCBH](-) fundamental modes suggests the nitrogen dioxide molecule prefers to react with the anion over the cation.