We report development of a first-principles, real-space Green's function method for calculation of Compton profiles in the impulse approximation. For crystalline Be, we find excellent agreement with prior theoretical treatments requiring periodicity; with prior experimental measurements of the Compton profile; and with new measurements of the dynamical structure factor via nonresonant inelastic x-ray scattering (often also called x-ray Thomson scattering in the plasma physics community). We also find good agreement with prior experimental results for the Compton profile of Cu. This approach can be extended to disordered and very high-temperature systems, such as 'warm dense matter', where theories presently used for the interpretation of inelastic x-ray scattering include condensed phase effects only at a perturbative level.2