The Oscar-winning actress 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.
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.
The Vietnamese authorities are only reported to have received Jolie's request for permission to adopt at the beginning of March.
Adoptions in Vietnam often take up to six months, but they can be fast-tracked if background checks and issues of whether the adopting family can support a child are quickly resolved.
In 2002 Jolie adopted her first child, Maddox, from Cambodia.
Three years later, she signed papers to adopt an Ethiopian baby called Zahara, who is now two.
She also has a biological daughter with partner Brad Pitt. Shiloh Nouvel Jolie-Pitt was born in Namibia last May.
In 2002 Jolie adopted her first child, Maddox, from Cambodia.
Three years later, she signed papers to adopt an Ethiopian baby called Zahara, who is now two.
She also has a biological daughter with partner Brad Pitt. Shiloh Nouvel Jolie-Pitt was born in Namibia last May.
Pitt later told US TV programme Today that becoming a parent was the "best thing" he had ever done.
Jolie filed adoption papers in Vietnam as a single parent, because the couple are not married.
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