When the Crimean War broke out in 1853 the Rifle Brigade sent two battalions. They fought at the Battle of the Alma, where one of their number led the advance across the river. The regiment also saw action at the Battle of Inkerman, and during the Siege of Sevastopol Victoria Crosses were awarded to members of the regiment over the course of the Crimean campaign.

During the campaign, the Rifle Brigade began to wear the softer forage cap in place of the more traditional shako.