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Catherine was accepted to study at Royal Holloway and Bedford New College, but became a stage manager at the Tricycle Theatre in London. She made her professional debut in Brendan Behan's play The Hostage before making her television debut in the BBC series Doctor Who in 1987. Part of a famous acting family, she is the daughter of Cyril Cusack and half sister of Niamh, Sinead and Sorcha Cusack - who also appeared in the programme in the role of Helen Connor in 2008.
Other TV and film credits include roles in Sophia and Constance, The Chief, The Bill, Cadfael, Ballykissangel, Boxed, Conspiracy of Silence, Jonathan Creek, Finding Neverland and Doctors, whilst on stage she has also performed in King Lear, Now Is The Hour, Les Liaisons Dangereuses, Agnes Of God, You Never Can Tell, The Seagull, Brighton Rock, The Glass Menagerie and Mill on the Floss.