Mr Sessions is under increasing pressure from the opposition after the Washington Post revealed how he failed to disclose his two conversations with the Russian ambassador Sergey Kislyak during the presidential campaign.
“Now, after lying under oath to Congress about his own communications with the Russians, the Attorney General must resign,” said Ms Pelosi.
“Sessions is not fit to serve as the top law enforcement officer of our country and must resign.
“There must be an independent, bipartisan, outside commission to investigate the Trump political, personal and financial connections to the Russians.”
Ms Pelosi, who infamously once said she could “guarantee” the 70-year-old billionaire would not become president, pointed to Mr Sessions’ confirmation hearing in January.
Mr Sessions, who was early an advocate of Mr Trump’s during his wild-card race for the White House, appeared to outright deny contact with the Russians.
Ms Pelosi, who made history when she became the first female speaker in The House, added: “Under penalty of perjury, he told the Senate Judiciary Committee, ‘I have been called a surrogate at a time or two in that campaign and I did not have communications with the Russians’.
“We now know that statement is false.”
In a response to Senator Al Franken of Minnesota, Mr Session's exact words were: "I didn't have, did not have communications with the Russians, and I'm unable to comment on it."
The 76-year-old, in a statement tweeted out yesterday, said Mr Sessions has “never had the credibility to oversee the FBI investigation of senior Trump officials’ ties to the Russians”.
Mr Sessions replaced acting Attorney General Sally Yates who refused to play along with Mr Trump’s immigration travel ban.
In a response this week, Justice Department spokeswoman Sarah Isgur Flores said Mr Session's response at the Senate was not misleading.
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