The vibrational behavior and the molecular dynamics of the high Tc superconductor Ba0.6K0.4BiO3 have been studied experimentally and by atomistic computer simulation methods. For Ba0.6K0.4BiO3, the vibrational spectrum is dominated by oxygen ion modes from 150cm-1 to 820cm-1 including infrared absorption bands at 330, 480, 640 and 830cm-1including infrared absorption bands at 330, 480, 640 and 830cm-1at room temperature. Band assignments are discussed in relation to those bands predicted by simulations, and the infrared and Raman measurements reported in the literature.