The couple, who secretly got married in 2011, is set to play adulterous pair named Robert and Emma, reported Aceshowbiz.
In the production which is directed by Broadway veteran Mike Nichols, Emma, who is married to Robert, is having an affair with Jerry, which will be portrayed by "Life of Pi" star Rafe Spall.
"Betrayal" previews from October 1 and opens on November 3 at New York's Barrymore Theatre.
"Betrayal", which is inspired by Pinter's affair with broadcaster Joan Bakewell, will mark a Broadway debut for Weisz.
Craig and Weisz were previously paired up as husband and wife in Jim Sheridan-directed psychological thriller "Dream House".
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