Following advice from doctors, the 76 year-old Hurt will no longer appear in the six week run of John Osborne's play, which will open in August.
The actor was cast as Billy Rice, a retired music hall entertainer, opposite Branagh, who will play Billy's son Archie Rice.
Hurt was recently hospitalised with an 'intestinal complaint', and has been advised by doctors not to continue with the show.
He commented: "Although I am much improved and on the road to a full recovery, my doctors have advised that it is too soon for me to undertake a lengthy and arduous stage role. It is therefore with great sadness and disappointment that I must withdraw from The Entertainer.
"I would like to send Ken, Rob and the entire company my love and very best wishes for a happy and successful production of a wonderful play."
Rob Ashford's production stars Phil Dunster as Graham, Jonah Hauer-King as Frank Rice, Crispin Letts as Brother Bill, Sophie McShera as Jean Rice and Greta Scacchi as Phoebe Rice.
A replacement for Hurt will be announced in due course.
The Entertainer runs at the Garrick Theatre from 30 August to 12 November.
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