With her 5-year-old son Maddox in tow, on Saturday she toured an Afghan Sikh refugee camp in New Delhi, listening to children play religious music and chatting with students, a UNHCR statement said.
Some 9,500 Afghan Sikh refugees are in India. They fled Afghanistan after the Taliban seized power in 1996 and targeted non-Muslims.
She also visited the one-room home where a refugee from Myanmar lives with her three children, it said.
The woman, one of the 1,750 refugees who have fled Myanmar to India since 1982, told Jolie that she and her children left after her husband was arrested by the military government in Myanmar, the statement said.
Myanmar-India relations turned cold after the Myanmar military violently suppressed pro-democracy demonstrations in 1988, but relations have warmed in the past few years.
"I am grateful to the refugee families who spent time with me and shared their stories. They are remarkable, courageous people," the statement quoted her as saying.
On Sunday, Jolie met Indian Junior External Affairs Minister Anand Sharma and lauded India's help to the refugees.
"The wonderful thing that I have learned since I have been in India is there are many, many needs for your own people and yet you have all been so gracious and been so open to so many refugees over the years," Jolie said in her first interaction with reporters since she arrived in India last month.
"I have also since I have been here spent time with Indian people and we spoke about concerns for disabled people, children and orphans," she said after meeting with Sharma.
Jolie is scheduled to return to the western Indian city of Pune to resume shooting this week for the film, "A Mighty Heart," in which she plays Mariane Pearl and Dan Futterman portrays Daniel Pearl.
A bungalow and adjoining cottages replicate the area Pearl and his wife stayed in Karachi before Pearl's abduction.
The Wall Street Journal reporter was abducted and murdered in Pakistan in 2002 while researching a story on Islamic militancy.
Pune is about 100 miles south of Mumbai, India's financial and entertainment hub.
The movie is based on an adaptation of Mariane Pearl's book, "A Mighty Heart: The Brave Life and Death of My Husband Danny Pearl," and is co-produced by Plan B, a production company founded by Brad Pitt and his ex-wife, actress Jennifer Aniston.