The Oscar-winning Actress Angelina Jolie collected the boy from a Ho Chi Minh City orphanage after a short and tearful farewell.
She is due to hold an official ceremony at the justice department later on Thursday, which will complete the adoption process.
Jolie, 31, has already adopted two children, from Cambodia and Ethiopia, and last year she gave birth to a daughter with actor partner Brad Pitt.
Jolie and Pitt visited Ho Chi Minh City last November, where they first met children at the Tam Binh orphanage.
She arrived in Vietnam again on Wednesday night, and early on Thursday morning she went to the orphanage, taking Maddox - her five-year-old Cambodian son - with her.
About 20 children dressed in traditional Vietnamese tunics welcomed the pair as they arrived.
Nguyen Van Trung, the director of the orphanage, said it was an emotional moment when she left with her new three-year-old son.
"They tried to make friends with the Vietnamese boy, who cried when he saw them because for him, they are strangers," he told reporters. "Jolie was very moved. Both of them tried to comfort the little boy," he added.
The child has been living at the orphanage since he was abandoned as a baby, but if all goes to plan officials have said that Jolie can take him home by the weekend.
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