Princess Ashraf, who played a key role in domestic and international politics, died at her home in Europe on Thursday, advisor Robert Armao said on Friday.
She was widely regarded as a talented diplomat and headed the Iranian delegation to the United Nations General Assembly for more than a decade.
The princess was also considered a powerful spokeswoman and ally for her brother, although she was loathed by religious fundamentalists.
After the Islamic revolution overthrew Shah Mohammad Reza Pahlavi, she supported initiatives related to reviving Iran's cultural, literary and artistic heritage from exile.
Signup to our newsletter and follow us on Facebook and Twitter!
She is survived by one son, Prince Chahram, and five grandchildren and great grandchildren.
Princess Ashraf "was thinking about Iran till the very last moments of her life and she passed away with hopes for her homeland's liberation," wrote her nephew Reza Pahlavi, the son of the late Shah Mohammad Reza Pahlavi, on his Facebook page.
Reza Pahlavi, who lives near Washington, wrote in Farsi that he was "deeply saddened" by his aunt's death.
"I have many memories from her since childhood up till today. In particular her concern over Iran's loss of its status after the Islamic Revolution and a beacon of hope which she always had in her heart for Iran’s freedom and dignity," the Facebook posting read.
The princess "made outstanding efforts in line with improving people's social life and advancing women's rights, social welfare and combating illiteracy in Iran as well as in the international arena," Pahlavi wrote.