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The former EastEnders actress and current Strictly Come Dancing champion will take on the role of Eliza Doolittle in the play, which was the basis of musical My Fair Lady.
Starring opposite Rupert Everett, Tointon will portray a London flower girl selected to be transformed into a lady by Everett's Professor Henry Higgins.
Commenting on the news, Tointon's former Strictly Come Dancing co-star Tina O'Brien told the PA: "That is great news. She will make the best Eliza, she will be brilliant."
Pygmalion opens at the Garrick Theatre on May 12, running until September 3.
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