That brought a sharp attack from the Bush administration, which has rejected direct talks with Damascus until its changes its ways.
"Unfortunately that road is lined with the victims of Hamas and Hezbollah, the victims of terrorists who cross from Syria into Iraq," said Gordon Johndroe, a spokesman for President Bush's National Security Council.
Washington accuses Syria of backing Hamas and Hezbollah, two groups it deems terrorist organizations.
It also says Syria is fueling Iraq's violence by allowing Sunni insurgents to operate from its territory and is destabilizing Lebanon's government. Syrian security officials have been implicated in the 2005 assassination of former Lebanese premier Rafik Hariri in Beirut, though Damascus has denied a role.
Pelosi was the highest-ranking American politician to visit Syria since relations began to deteriorate in 2003.
Then Secretary of State Colin Powell went to Damascus in May 2003.
The visit heightened tensions between the administration and congressional Democrats, who have stepped up their push for change in U.S. policy in the Mideast and the Iraq war. But Democrats - and some Republicans - say the refusal of dialogue has closed doors to possible progress in resolving Mideast crises.
"We came in friendship, hope, and determined that the road to Damascus is a road to peace," said Pelosi, who met for three hours with Syrian President Bashar Assad.