The House Ethics Committee on Thursday found “substantial evidence” that Representative George Santos violated federal law, setting the stage for another push to expel the embattled first-term Republican from New York and prompting him to declare that he would not seek re-election.

House investigators found evidence that Mr. Santos used campaign funds for personal purposes, defrauded donors and filed false or incomplete campaign finance and financial disclosure reports, according to a 56-page report released on Thursday.

The committee voted unanimously to refer its findings to the Department of Justice, saying that Mr. Santos’s conduct “warrants public condemnation, is beneath the dignity of the office, and has brought severe discredit upon the House.”

And while the panel refrained from recommending any punitive measures, there were already indications that the report could be the catalyst for a third effort to remove Mr. Santos from office. Numerous House members have previously said that they would support his expulsion if the committee found criminal wrongdoing or a severe breach of ethics.

“Most of us have never seen anything like this — this extensive, this brazen, and this bold,” said Representative Glenn F. Ivey, Democrat of Maryland, who sits on the Ethics Committee.

Mr. Ivey, a former federal prosecutor, said he believed the panel’s staff had uncovered additional evidence that could be used in Mr. Santos’s federal prosecution.

Mr. Santos, 35, a Republican representing parts of Long Island and Queens, already faces a 23-count federal indictment that includes accusations that he stole from his donors and falsified election campaign filings. Mr. Santos, who did not immediately respond to a request for comment, has resisted calls for his resignation, and has pleaded not guilty.

Shortly after the report was released, Mr. Santos announced on X, the website formerly known as Twitter, that he would not seek re-election in 2024. Even so, he appeared to take issue with the findings of the committee, writing: “If there was a single ounce of ETHICS in the “Ethics committee,” they would have not released this biased report.”

Ethics investigators concluded that Mr. Santos “sought to fraudulently exploit every aspect of his House candidacy for his own personal financial profit,” the report said, noting that he sustained his campaign “through a constant series of lies to his constituents, donors, and staff about his background and experience.”

Mr. Santos reported hundreds of thousands of dollars in fictitious loans to his campaign, the report said, then repaid himself with real money.

The report also detailed how Mr. Santos submitted numerous expenditures that did not appear to have a campaign purpose, from travel and hotel stays in Las Vegas that corresponded to the time when he was to have been on his honeymoon, to thousands of dollars at spas. At least two payments were described as being for Botox.

Some of the most salacious details of the report concern a company called RedStone Strategies, which Mr. Santos used to raise money without being subjected to campaign contribution limits.

Investigators found that Mr. Santos transferred at least $200,000 to himself from RedStone spread over numerous transactions in 2022. That money was then used to pay off personal credit cards, make purchases at Hermes and Sephora, and spent on OnlyFans, a website known for its adult content.

The committee was not able to substantiate accusations that Mr. Santos was guilty of sexual harassment. The allegations were made last February by a prospective aide who accused Mr. Santos of coming onto him, then firing him after his advances were rebuffed. The Santos team said that the aide had been fired after it learned of wiretapping charges the man faced in Ohio.

Earlier this month, a bloc of first-term Republicans representing moderate districts in Mr. Santos’s home state of New York forced a vote on his expulsion from Congress. That effort failed decisively, with many House members saying they were leery of setting a precedent for removal without a finding from a court or the Ethics Committee.

Those critics, led by Anthony D’Esposito, a fellow Long Island Republican, have wasted little time in using the ethics report to push their colleagues on both sides of the aisle to reconsider Mr. Santos’s expulsion.

Representative Dan Goldman, Democrat of New York, said in a statement that he would file a motion to expel Mr. Santos from the House after Thanksgiving.

Luke Broadwater and Michael Gold contributed reporting.

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