A nearly 22-hour debate in the Senate closed with an overwhelming 55-22 vote against Brazil's first female president. Pro-impeachment senators broke into applause and posed for selfies and congratulatory group photos in the blue-carpeted, circular chamber.
Only a simple majority of the 81-member Senate had been required to suspend Rousseff for six months pending judgment on charges that she broke budget accounting laws. A trial could now take months, with a two-thirds majority vote eventually needed to force Rousseff, 68, from office altogether.
He was preparing to announce a new government shortly and said his priority is to address Brazil's worst recession in decades and end the paralysis gripping Congress during the battle over Rousseff.
"He will inherit much of Brazilians' dissatisfaction with the political tradition that he embodies," said Thiago Bottino, an analyst at the Getulio Vargas Foundation.
A onetime Marxist guerrilla tortured under the country's military dictatorship in the 1970s, Rousseff has denounced the impeachment drive as a coup and vowed to fight on during her trial.
A crowd of supporters was gathering outside the presidential palace to salute her as she drove off, a spokesman for the Workers' Party told AFP.
She was expected to go to her official residence where she will continue to live with her mother during the impeachment trial. She will retain her salary and bodyguards.
The leader of the Workers' Party in the Senate, Humberto Costa, said his side would now work to convince senators to support Rousseff in the trial and turn the tide in her favor.