The syntheses, IR and Raman spectra of four nanosize giant cluster compounds were reported in this paper. These compounds show similar IR and Raman spectra because they were assembled by the similar building blocks. The bands with frequencies in IR spectra in the range from 980 to 550 cm-1 and those absorptions under 970 cm-1 in Raman spectra have to be attributed to the absorptions of Mo-O bonds including Mo = O, Mo-O-Mo and mu 3-O-Mo bonds.