FT-IR and μ-Raman spectra of 4-chloro-3-nitrobenzonitrile have been recorded in the range of 400-4000cm-1 and 100-4000cm-1, respectively. It has been prepred from the reaction of 4-chloro-3-nitrobenzamide and phosphorus oxychloride. Crystal structure of 4-chloro-3-nitrobenzonitrile has been reported. Molecules of 4-chloro-3-nitrobenzonitrile are linked by weak intermolecular C-H…O and C-H…N hydrogen bonds.