The Infrared and Raman spectra of 4-Phenylpyridine are reported for the first time in the 4000-400cm−1range. Vibrational assignments have been made for fundamental modes on the basis of frequency shifts of coordinated legend, infrared and Raman band contours and comparisons with the assignments for related molecules. The infrared spectra of M (4-Phenylpyridine) Ni(CN)4complexes (M=Mn, Ni or Cd) are reported. Their structure consists of polymeric layers of [M-Ni(CN)4]∞with the 4-phenylpyridine molecules bound to metal (M), similar to the structure found in Hoffmann type host complexes.