The viral campaign aims to publicise the unlawful activity of guerrilla group leader Joseph Kony in Uganda.
A documentary titled Kony 2012 was launched by action group Invisible Children last week, in order to draw attention to Kony, who is said to have abducted many children and place them into his army by force.
Jolie said that she didn't "know anyone who doesn't hate Kony" at an event to mark International Women's Day in New York.
The actress - who is also a Goodwill Ambassador for the United Nations - said: "I've been to Uganda and Congo and been to the international criminal court myself... he's the one we all want to see in jail, so I think it's great that more people are talking about it.
"He's an extraordinarily horrible human being who, you know... his time has come and it's lovely to see that young people are raising up as well."
Jolie was named as one of a list of 20 "culture-makers" that the Kony 2012 video creators hoped would lend their support and contributions.
Rihanna and Taylor Swift have also spoken out against Kony after the video was uploaded to YouTube.
Filmmaker Jason Russell has defended the film against critics since its release. He had originally hoped the video would reach 500,000 views, but has so far hit over 74 million hits.
> Speech Debelle on Kony 2012 campaign: "I can't be a part of it"
Watch the documentary below: