The 23-count superseding indictment also includes charges such as wire fraud, making false statements to the Federal Election Commission, and money laundering.
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The charges follow the indictment last week of Santos' former campaign finance chief Nancy Marks.
Santos walked out of the closed-door meeting on Capitol Hill Tuesday night to a flood of cameras and reporters, saying he will fight the new charges "until the bitter end."
"I'm just going to look at - look, you're all acting like I'm not entitled to due process, and innocent until proven guilty," Santos said.
When asked about his next steps, Santos said "Nothing! I'm just going to go defend myself. I have a court date on August 27 to October 27, and then there's probably going to be something else scheduled after that, I'm entitled to due process, I'm going to defend myself."
When asked if he would resign, Santos said, "I will not."
Together prosecutors said they enlisted 10 family members without their knowledge to donate to the campaign to make it seem like Santos was getting enough support to qualify for party funds.
According to the charges, Santos said he had loaned his campaign $500,000 in an attempt to convince Republican Party officials that he was a serious candidate, when he actually had less than $8,000 in his personal accounts.
"As alleged, Santos is charged with stealing people's identities and making charges on his own donors' credit cards without their authorization, lying to the FEC and, by extension, the public about the financial state of his campaign," U.S. Attorney Breon Peace said in a statement.
Rep. Santos' lawyer declined to comment when asked by ABC News.
The new charges include allegations that he charged more than $44,000 to his campaign over a period of months using cards belonging to contributors without their knowledge. In one case, he charged $12,000 to a contributor's credit card and transferred the "vast majority" of that money into his personal bank account, prosecutors said.
Santos is due back in court on October 27.
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The indictment came on the same day that Long Island Democrat Tom Suozzi launched a campaign to retake the New York congressional seat held by Rep. Santos.
The new charges deepen the legal peril for Santos, who likely faces a lengthy prison term if convicted. So far, he has resisted all calls to resign, insisting he intends to run for reelection next year.
Santos' personal and professional biography as a wealthy businessman began to unravel soon after winning election to represent Long Island and Queens last year, revealing a tangled web of deception.
In addition to lying to voters - about his distinguished Wall Street background, Jewish heritage, academic and athletic achievements, animal rescue work, real estate holdings and more - Santos is accused of carrying out numerous fraud schemes meant to enrich himself and mislead his donors.
He was initially arrested in May on a 13-count federal indictment, which charged him with using funds earmarked for campaign expenses on designer clothes and other personal expenses and improperly obtaining unemployment benefits meant for Americans who lost work because of the pandemic.
Free on bail while awaiting trial, Santos has described his litany of lies as victimless embellishments, while blaming some of his financial irregularities on his former treasurer, Nancy Marks, who he claims "went rogue."
Last week, Marks, a longtime Long Island political bookkeeper and close aide to Santos, pleaded guilty to a fraud conspiracy charge, telling a judge that she helped her former boss hoodwink prospective donors and Republican party officials by submitting bogus campaign finance reports.
Tuesday's indictment said Marks and Santos were involved in the same scheme to fake a $500,000 campaign loan in order to meet a benchmark that would unlock additional support from a Republican Party committee. Santos has now also been charged with recording fake donations from at least 10 people, all his or Marks' relatives, as part of the same effort to make the campaign look like it hit those fundraising goals.
Santos said he has not had contact with Marks.
"I had a phone call - I had a phone call with who I had to have a phone call with. But now I am going to go home and see what this is all about and it's not surprising I wouldn't be the first or the last to have this happen so," Santos said.
Santos was not initially charged in the criminal complaint against Marks, but was identified in court papers as a "co-conspirator."
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The new indictment alleges a multi-part fraud by Santos, who allegedly duped both his donors and his family members.
In one instance, Santos allegedly swiped the credit card information of one of his contributors, who had already donated $5,800 to the campaign, to give himself an additional $15,800 in payments, the indictment said. Because the unauthorized charges exceeded contribution limits under federal law, Santos listed the additional payments as coming from his own unwitting relatives, prosecutors allege.
Financial questions have continued to swirl around Santos, who claimed to be rich but spent much of his adulthood bouncing between low-paying jobs and unemployment, while fending off eviction cases and two separatecriminal charges relating to his use of bad checks.
A separate fundraiser for Santos, Sam Miele, was also previously indicted on federal charges that he impersonated a high-ranking congressional aide while soliciting contributions for the Republican's campaign.
Prosecutors said Miele, 27, impersonated the former chief of staff to GOP Rep. Kevin McCarthy, who at the time was the House minority leader, by setting up dummy email addresses that resembled the staffer's name.
Miele's attorney, Kevin Marino, previously predicted his client would be exonerated at trial.
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Information from ABC News and the Associated Press