Mineral liberation is one of the primary objectives in comminution circuits for the downstream separation of valuable minerals. Breaking minerals through their grain boundaries (grain-boundary breakage) enables mineral liberation in their natural grain size, removing the need for intensive grinding. This study aimed to evaluate if gaseous carbon dioxide, oxygen, or hydrogen can be used as grinding additives to promote the liberation of chromite grains by grain-boundary breakage. For this purpose, chromite ore particles in the -9.53 + 6.35 mm size fraction were pretreated by exposing them to carbon dioxide, oxygen, or hydrogen flow. Then, the untreated and pretreated samples were broken in a drop-weight tester under the same conditions. Finally, the grade-recovery plots of chromite grains in the selected progeny size fractions and the overall progeny distributions were measured and compared. Pretreatment with carbon dioxide flow was found beneficial for grain-boundary breakage. It significantly enhanced the liberation of coarse chromite grains along with the overall progeny fineness. EPMA analysis showed that the adsorption of carbon dioxide seems to reduce aluminum concentration at grain boundaries, which could be the reason for grain-boundary weakening. These results suggest that carbon dioxide can be used as a grinding additive, reducing the carbon footprint of the mining industry.