"Trump is goading us to impeach him," she said at an event in New York City hosted by the Cornell University Institute of Politics and Global Affairs. "That's what he's doing. Every single day, he's just like taunting, taunting, taunting because he knows that it would be very divisive in the country, but he doesn't really care. He just wants to solidify his base."
House Democratic leaders, including Pelosi, have worked to tamp down talk of impeachment for months. Pelosi has consistently emphasized that impeachment is extremely divisive, and in March she said Trump is "just not worth it."
But while she has taken a cautious approach to the issue of impeachment, Pelosi has also been quick to defend congressional oversight of the administration and appears to be publicly growing frustrated with stonewalling from the White House.
Pelosi reiterated on Tuesday that she wants to continue with the process of gathering more information, saying "we have to see where the facts take us" and warning that Democrats will "be ready" for whatever may come.
And Pelosi again argued that Trump is obstructing justice, pointing to the White House refusing to comply with subpoenas.
"Every day, he's obstructing justice by saying this one shouldn't testify and that one shouldn't testify and the rest. So he's making the case, but he's just trying to goad us into impeachment. And wherever you go, I say to my colleagues, whatever it is, be ready. And whatever it is, we'll be ready."
Pelosi was asked whether proceeding with impeachment might help Democrats in expected court battles in response to White House stonewalling.
The speaker reiterated that Democrats still need to be able to gather "more information" and emphasized the importance of obtaining the full, unredacted Mueller report, but cautioned that "one thing leads to another."
"One thing leads to another," she said. "One hearing leads to another, where they don't tell the truth ... and that might take us to a place. We have to have more, I believe we have to have more information. But our impeachment power is a justification for our getting that other information."
Pelosi rebuts McConnell: 'the case is not closed'
Pelosi also had a message for Senate Majority Leader Mitch McConnell on Tuesday: "The case is not closed."
Pelosi referenced McConnell's remarks earlier in the morning where he argued that it's time to move on from Mueller's investigation and report, declaring "case closed."
"I don't think so. I don't think so," Pelosi said. "Just as a matter of observation, that's just not a fact. The case is not closed."
Pelosi and Senate Democratic leader Chuck Schumer later released a statement criticizing the Senate's top Republican over his statement.
"Senator McConnell's declaration of 'case closed' is a stunning act of political cynicism and a brazen violation of the oath we all take," the congressional Democratic leaders said in a joint statement, saying that the Mueller report "left a raft of unanswered questions about coordination between the President's campaign and Russia. These are not trivial or political questions -- they go to the wellspring of our democracy. When a President is allowed to violate the law with impunity, and when a foreign power is allowed to interfere in our elections, it gnaws at the roots of the great oak that is our democracy, and could very well topple it."
During the event where she spoke on Tuesday, Pelosi broadly defended Democratic oversight of the administration and brought up Russian interference in US elections, saying, that "should be a cause of action for every branch of government."
Pelosi added, "the facts, the data, the evidence, the truth is what we want to base our decisions on and the administration should be willing to share that unless they have something to hide and that's what we will find out."
CNN's Veronica Stracqualursi contributed to this report.
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