Hiddleston is to take on the role of Robert, one of four characters in Betrayal, which tells the story of an extramarital affair in reverse chronological order.
The play will run from March to June 2019 at Pinter's namesake theatre in the West End.
It will come as part of Jamie Lloyd's Pinter at the Pinter season, during which all of Pinter's short works are being played to mark the 10th anniversary of the Nobel-Prize-winning playwright.
Tickets sales will open on 30 November.
“Betrayal is a masterpiece," Hiddleston told London Theatre. "Jamie Lloyd’s Pinter at the Pinter season is terrific and I am so pleased that he’s asked me to be part of it.”
In addition to his Hollywood career, which as seen him gain acclaim as Loki, Thor's belligerent brother in the Marvel Universe, Hiddleston is an accomplished theatre actor.
His performance in Cymbeline earned him the Laurence Olivier Award for Best Newcomer in a Play in 2008.
That year, he earned an additional nomination in the same category for his role in Othello.
Hiddleston has also appeared in Ivanov and Coriolanus at the Donmar Warehouse, as well as The Children's Monologues at the Old Vic Theatre.
On Wednesday, the actor shared a cryptic teaser for Betrayal in a rare tweet.
He can be seen in the clip staring in the distance, visibly in turmoil.
Betrayal, which premiered in 1978, tells the story of two couples: Emma and Robert, and Robert's close friend Jerry and his own wife Judith (who never appears on stage).
The first scene takes place after the affair between Emma and Jerry has ended and goes back in time until its beginning.
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