Miller, who is well known for her roles in Layer Cake and American Sniper will play Maggie. Her previous theatre credits include As You Like It at Wyndham's, and Flare Path at Theatre Royal Haymarket.
O'Connell will play Brick. The actor has performed plays at the National Theatre and Royal Court, and is best known for playing James Cook in Skins. He was last seen on stage last year in The Nap at Sheffield Crucible.
The production will be directed by Benedict Andrews (A Streetcar Named Desire) and produced by the Young Vic. It is the first Young Vic production to debut in the West End following transfers including A View from a Bridge, Golem and The Scottsboro Boys.
Cat on a Hot Tin Roof won Williams the 1955 Pulitzer Prize for Drama, and is about a family gathering in Southern America and how Brick and wife Maggie interact with the rest of the family.
Cat on a Hot Tin Roof will run at the Apollo Theatre from 24 July to 7 October, with previews from 13 July.
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