In this paper, the characteristic vibrational modes of aniline were analyzed using polarized Raman and two-dimensional Raman correlation spectroscopy methods. Polarized Raman spectra revealed the presence of anomalous phenomena in the ring-breathing and C-H vibrational modes of aniline. The symmetry and asymmetry vibrational properties of these vibrations were fully manifested in the polarized Raman spectrum. In the case of N-H vibrations, the results that are usually observed were determined. To explain the anomalies observed in the polarized Raman spectra, two-dimensional Raman synchronous and asynchronous spectra were generated based on Raman spectral data of aniline in ethyl acetate at various concentrations. These spectra strongly supported the conclusions drawn from the polarized Raman spectra.