"He's so hard to buy for," Jolie told staff members at the home during their private viewing at the time.
"Brad said he had a visual sense of Fallingwater, but experiencing it in person, hearing the sound of the waterfall cascading under the house and smelling the wood from the fireplace, was better than anything he could have imagined," said Fallingwater curator of education Cara Armstrong of architecture buff Pitt's visit.
The Moneyball star has expressed his love of architecture in the past. "While acting is my career, architecture is my passion," Pitt was once quoted as saying.
"Brad has always loved Fallingwater and his first trip there was unforgettable," a source told the Mail.
"Angelina wanted to get him something incredibly special and, because she knows how much he loves architecture, she thought this would be perfect.
"Brad has dreamed of a home with the sound of a waterfall cascading under the house," the source continued. "Brad has always wanted to design his own house. He wants to pull all aspects of nature, light, glass and varying levels into the concept."
And Jolie's timing is right on the money. The pair, who raise six kids together, recently sold their four-bedroom, four-bath, 4000 square foot beachfront Malibu abode to Ellen DeGeneres and wife Portia de Rossi for a cool $12M.
Plenty of coin for chasing waterfalls.
In other Jolie-Pitt news...
Jolie reveals in a recent interview that Pitt is a bit of a "pushover" when it comes to their children.
"In our house, we're split 50-50," Jolie tells The Chicago Sun Times. "I will say, 'Brad, you can't just give the girls anything they want'. He will look at me, smile, and say, 'I have no choice. My girls are perfect'."
She added: "Brad has called me on things too. He said, 'Angie, you let the boys walk all over you'. The truth is I do. Boys can push a mum. Girls can't.
"Maybe that's because women know women. We know little girls. I'll say, 'Girls, I know exactly what you're doing. You're working Daddy for that cookie'. Men can never say no."
The In the Land of Blood and Honey director also praised Pitt for his parenting skills.
"Brad shows my girls how a woman should be treated by a man," she adds.
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