The daughter of Mr. and Mrs. Robert Cassidy, Catherine Calvert was born and raised in Baltimore, Maryland.

She made her stage debut in the play Brown of Harvard in September 1908, in Albany, New York. On Broadway, she portrayed Laura Moore in The Deep Purple (1911), May Joyce in The Escape (1913), and Dona Sol in Blood and Sand (1921).

After many years' experience onstage in productions including The Deep Purple (a play by her future husband, Paul Armstrong), in 1910, she entered films via Keeney Pictures Corporation in A Romance of the Underworld (1918; based on a play in which she had appeared onstage).

Other films in which she appeared include Marriage, Out of the Night, Career of Katherine Bush, Marriage for Convenience, and Fires of Faith. Around 1920 she was a star of Vitagraph Studios.

Calvert married Paul Armstrong in New Haven in 1913. They remained wed until his death in 1915. She later married Canadian grain exporter George A. Carruthers.

In 1971, Calvert died in Uniondale, New York, at age 80.