The phonon density of states ͑DOS͒ gives insight into interatomic forces and provides the vibrational entropy, making it a key thermodynamic function for understanding alloy phase transformations. Nuclear resonant inelastic x-ray scattering and inelastic neutron scattering were used to measure the chemical dependence of the DOS of bcc Fe-Co alloys. For the equiatomic alloy, the A2 → B2 ͑chemically disordered→ chemically ordered͒ phase transformation caused measurable changes in the phonon spectrum. The measured change in vibrational entropy upon ordering was −0.02Ϯ 0.02 k B /atom, suggesting that vibrational entropy results in a reduction in the orderdisorder transition temperature by 60Ϯ 60 K. The Connolly-Williams cluster inversion method was used to obtain interaction DOS ͑IDOS͒ curves that show how point and pair variables altered the phonon DOS of disordered bcc Fe-Co alloys. These IDOS curves accurately captured the change in the phonon DOS and vibrational entropy of the B2 ordering transition.