He left school at the age of 14 to become a stage actor, and three years later, traveled to the United States to begin working on Broadway, starring in The First Born in 1897.

Bryant starred in A Train of Incidents (1914) and War Brides (1916), which was the first film of his wife Alla Nazimova.

Bryant and Nazimova signed with Metro Pictures in 1918 and starred alongside each other in a number of films including Revelation, Out of the Fog, and Billions.

Salomé was notably too far ahead of its time and failed at the box office, bankrupting Nazimova Productions.

When the press uncovered the fact that Charles had listed his current marital status as "single" on his marriage licence, the revelation that the marriage between Alla and Charles had been a sham from the beginning embroiled Nazimova in a scandal that damaged her career.