Naturally occurring Al- Fe3 +- poor magnesiochromite and Fe2+- Fe3 +- rich ferrian chromite solid solutions have been analyzed by micro-Raman spectroscopy. The results reflect a strong positive correlation between the Fe3 + # [Fe3+/(Fe3 ++Cr + Al)] and the positions of all Raman bands. A positive correlation of the Raman band positions with Mg# [Mg/(Mg + Fe2 +)] is less stringent. Raman spectra of magnesiochromite and ferrian chromite show seven and six bands, respectively, in the spectral region of 800 − 100 cm− 1. The most intense band in both minerals is identified as symmetric stretching vibrational mode, ν1(A1g). In the intermediate Raman-shift region (400–600 cm− 1), the significant bands are attributed to the ν3(F2g) > ν4(F2g) > ν2(Eg) modes. The bands with the lowest Raman shifts (< 200 cm− 1) are assigned to F2g(trans) translatory lattice modes. Extra bands in magnesiochromite (two bands) and in ferrian chromite (one weak band) are attributed to lowering in local symmetry and order/disorder effects.