The Salt actress is said to have purchased the piece of land in California so that Pitt can build a home in the vein of American architect Frank Lloyd Wright's Fallingwater.
"Brad has always loved Fallingwater and his first trip there was unforgettable," a source told the Daily 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 insider 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."
Pitt recently insisted that he chooses only quality projects in order to ensure the longevity of his career, claiming that movies should age like a "fine wine".
In December, Jolie said that Pitt played a key role in helping her develop her directorial debut In the Land of Blood and Honey.