Jolie brief the council as special envoy for the UN on refugee issues.
Syria's ambassador said simply of her presence, "She's beautiful."
Nearly four million Syrians have fled the conflict into neighboring countries, which warn they are dangerously overstretched.
"We cannot look at Syria, and the evil that has arisen from the ashes of indecision, and think this is not the lowest point in the world's inability to protect and defend the innocent," Jolie said.
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Jolie, who said she has made 11 visits to Syrian refugees in the region since the crisis began in 2011, called strongly for the political will to act.
Russia, a top Syria ally and backed by China, has vetoed multiple council resolutions on Syria, including an effort last year to refer the situation there to the International Criminal Court.
Jolie said the council must now "work as one," and she said she would like to see the foreign minister of each of the 15 council members come to the table to negotiate a political solution.
In addition, Jolie spoke briefly about the rising migrant crisis on the Mediterranean, where more than 1,300 migrants fleeing Syria and other places have drowned at sea over the past three weeks.
"It is sickening to see thousands of refugees drowning on the doorstep of the world's wealthiest continent," she said. "No one risks the lives of their children in this way except out of utter desperation.