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Harman, who played Dennis Rickman in the BBC soap, will take on the role of Lord Farquaad in the West End production.
The title role of Shrek will be played by Four Lions star Nigel Lindsay, BBC News reports.
The production's producers Bill Damaschke and Caro Newling said that the actors "blew us away with their audition performances". They are continuing to cast a further 28 roles.
In July, it was announced that Amanda Holden and RIchard Blackwood had signed on as Princess Fiona and Donkey respectively.
Shrek: The Musical is scheduled to open at the Theatre Royal on Drury Lane in May 2011.
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