The energy bands, density of states and Compton profile of Cr2S3 have been computed using band structure methods namely linear combination of atomic orbitals with density functional theory as well as by spin polarized relativistic Kronig–Kramer–Rostokar method. To analyze the theoretical data on electron momentum densities, the Compton profile of Cr2S3 has been measured using 100mCi 241Am Compton spectrometer. The isotropic profile satisfies the calculated profiles. The band structure calculations are also compared with the available data.