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An Italian actor was cast as Victoria (Elizabeth Debicki)'s husband, Alexander. Making his starring English-language feature debut as the handsome race car driver is Italian Luca Calvani. Calling him a new discovery for worldwide audiences, producer Lionel Wigram commented: "Luca is the epitome of what we had in mind. He gives Alexander just the right air of sinister glamour that makes him credible and, at the same time, so much fun."
Napoleon Solo's trick of removing a tablecloth from a table while leaving all the objects undisturbed was not a visual effect. Henry Cavill actually performed it himself, having been trained in the trick by British variety star Mat Ricardo.
Henry Cavill and Armie Hammer often performed their own stunts. Hammer was more enthusiastic about his stunts, to the point that his stunt double joked that he hardly had a chance to do anything because he was out there doing it all by himself.
Henry Cavill admitted that he was very relieved to not have a shirtless scene in this movie after a string of movies where he had to be in top shape. Cavill said that he was glad to focus on his performance for once and not his physique, which he said took an enormous amount of work to present on screen.
Armie Hammer watched The Man from U.N.C.L.E. (1964) before starting production to prepare for his role as Illya Kuryakin. He was the only member of the cast to do so.
Armie Hammer confessed to being awed by co-star Henry Cavill upon first meeting him. Hammer recalled, "I was overwhelmed by his good looks, his chiseled body, his muscles, pretty much everything. There was the whole package there."
David Beckham: as the projectionist at the beginning of the movie, when Illya is being briefed about Solo.