She first became famous after playing the lead in a 1962 BBC adaptation of What Katy Did. Soon afterwards, she was taken up by Walt Disney, and starred in The Three Lives of Thomasina and The Fighting Prince of Donegal. Her appeal was that of an "English rose", and few people were aware of her problem with dyslexia. In her autobiography, Susan's Story, she publicised her experiences, and her work on behalf of dyslexics eventually led to her being awarded the O.B.E.
Susan Hampshire appeared in several long-running television serials, notably in the BBC's blockbuster, The Forsyte Saga (1967), in which she played Fleur. In 1969, she starred as Sarah Churchill in The First Churchills, and in 1974, she played the lead in another 26-part serial, The Pallisers. She currently stars in Monarch of the Glen.