Abstract: In order to study Raman spectral characteristics of ammonium thiocyanate solution,geometry of SCN- was optimized based on 6-31G(d) basis set and its Raman spectra was calculated using Hartree-Fock (H-F)method. The Raman spectra of ammonium thiocyanate solution with different concentrations were measured experimentally. It was found that the relationship between the concentration of SCN- and the corresponding Raman peakintensity waslinear.The results show that absolute error and relative error of the experiment result(752cm-1)and the theoretical calculation (740cm-1) of Raman vibrationalfrequency of SCN- is a little. However,envelopes appear in another Raman region.The resultsprovide a help for measurement of ammonium thiocyanate solution withdifferent concentrations inindustry.