Aside from filming intense arguments with Pitt as their characters, Vanessa and Roland, in the '70s drama -- during what was technically their honeymoon -- the 40-year-old Oscar-winning actress says shooting their sex scenes was even weirder.
"It’s the strangest thing in the world to be lying naked in a bathtub with an iPad that’s showing you the shot outside, while your husband is at the door and you're directing him to come in and make love to you," Jolie tells Entertainment Weekly. "In front of a bunch of other men with cameras."
She admits that Pitt, 51, was more than a little protective of her.
"I couldn't get out of the bathtub to get to the monitor because the director is naked," she laughs. "We're artists and want to be free, but Brad -- it's his wife. He was on towel duty. He'd hold the towel over me."
"Love scenes are strange anyway, but when you're doing a love scene with a person that you really have sex with? The only way to get through it was for us to all talk about the absurdity of it and make sure no one was feeling awkward," she adds. " ... I've done sex scenes. But this is obviously different. I almost wish every woman could have this experience."
On a more serious note, Jolie hopes her topless bathtub scene will give confidence to other women who have had a mastectomy. The actress had previously admitted to The New York Times that she didn't want to do the nude scene because of insecurities about her body, particularly after undergoing a preventative double mastectomy in February 2013.
"The surgeries still allow you to be a woman," Jolie stresses. "I hope other women -- anyone who is worried about those issues and how [your body] can feel or look -- can see that through [the scene]. I’m happy that will be in there if that answers something for them."
Though it wasn't always so serious on the set. Jolie reveals some of the "crazy" antics she and Pitt improvised as their characters.
"Brad and I had this one day when we were like, 'Let's just do ridiculous things and see what happens,'" she explains. "By the end of it, he had pissed all over my shoes, I had packed up the entire [hotel] room to leave, and he wrote "pillhead" with an arrow on my head with a Sharpie while Vanessa was sleeping."
"The crazy stuff didn't make it into the film," Jolie laughs. "It went awry."
Watch the video below to see how their daughter, 9-year-old Shiloh Jolie-Pitt, pranked her dad on set!