Infrared and Raman spectra are reported for two new metal diisoquinoline tetracyanonickelate complexes of the form M(isoquinoline)2Ni(CN)4 where, M=Ni or Cd. It is proposed that their structure consist of two dimensional polymeric layers formed with Ni(CN)4 ions bridged by M(isoq)2 Cations. The isoquinoline molecules lie above and below the layers. Several modes of coordinated isoquinoline have upward wavenumber shifts in comparison to liquid phase values and the shifts are metal dependent. These are thought to be due to the coupling of the internal modes of the isoquinoline with the M-N vibrations.