New HofmannTd-type clathrates of the forms Cd(CPA)2M(CN)4.C6H6 (CPA = cyclopropylamine; M?Cd or Hg) prepared in powder form and characterized by FT-IR, FT-Raman, far-IR spectra, X-ray diffraction, and elemental analyses are reported. Vibrational assignments are proposed for the bands of the host lattice and guest molecule. It is shown that the spectra are consistent with a proposed crystal structure for the compounds derived from X-ray diffraction measurements. The C, H, and N analyses were carried out for all the compounds. All the vibrational modes of coordinated CPA are characterized. The spectral features suggest that these compounds are similar in structure to the HofmannTd-type clathrates.