Toomey said on Sunday that President Donald Trump, a fellow Republican, should resign after his supporters stormed the U.S. Capitol in a deadly rampage last week.
Toomey, who has been a supporter of Trump until recently, became the second Senate Republican to call for the president to step down.
"I think the best way for our country is for the president to resign and go away as soon as possible," he said in an interview with NBC's "Meet the Press."
Toomey said he did not think there was time for an impeachment with only 10 days left before Democrat Joe Biden is sworn in as Trump's successor. He told CNN's "State of the Union" he thought resignation was "the best way to get this person in the rear view mirror."
U.S. Senator Lisa Murkowski said on Friday that Trump should resign immediately and suggested she would consider leaving the party if Republicans cannot part from him.
Fellow Republican Senator Ben Sasse, a frequent Trump critic, told CBS News he would "definitely consider" impeachment because the president "disregarded his oath of office."
Toomey, a conservative who plans to retire at the end of his term in 2022, said he believed Trump had descended into a level of "madness" after the election that was unthinkable.
"I don't think there's any doubt at all ... that the president's behavior after the election was wildly different than before. He descended into a level of madness and engaged in activity that's just absolutely unthinkable and unforgivable," Toomey told CNN.
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