Raman scattering experiment and density functional theory calculation have been applied to investigate the vibrational modes of perovskite (C6H5CH2NH3)2PbBr4 in the spectral range of 450～1 700 cm-1. Comparing the experimental Raman spectrum and theoretical calculated result, it was found that density functional theory can be well applied to simulate the vibration modes oforganic part of (C6H5CH2NH3)2PbBr4. Furthermore, the origins of the observed Raman peaks in the spectral range of 450～1 700 cm-1 have been assigned by comparing the results of density functional theory calculation and literature reports. In addition, it was found that the Raman peaks in this spectral range are mainly originated from the vibrational modes of organic part of (C6H5CH2NH3)2PbBr4.