Witt is also accused in the Washington, DC, indictment of conducting research about her intelligence colleagues and using that data to draft "target packages" against them.
The charging documents outline a series of electronic messages between Witt and Individual A, who resided primarily in Iran, before she defected.
They declined to say to what extent these disclosures compromised US intelligence operations targeting Iran.
"She chose to turn against the United States and shift her loyalty to Iran", said Jay Tabb, the FBI's executive assistant director for national security.
She defected to Iran in 2013 after being invited to two all-expense-paid conferences in the country that the Justice Department says promoted anti-Western propaganda and condemned American moral standards.
According to authorities, Witt collaborated with Iran's Islamic Revolutionary Guard Corps, an elite military unit charged with exerting Tehran's influence around the world. Witt replied with a smiley emoticon, "LOL thank the sec of defense?"
The publication of the indictment coincided with the Treasury Department's announcing a new series of cyber-security related sanctions on a number of Iranian individuals and entities, including the IRGC, which engages in "efforts to recruit and collect intelligence from foreign attendees [of various conferences], including USA persons, and four associated individuals", according to the a release announcing the sanctions.
The next year, she went to another Iranian conference and soon arranged to defect, according to the indictment. She was a Defense Department contractor at the time.
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The hackers, using imposter Facebook personas, then targeted those same officials and were even able at one point to join a private Facebook group composed primarily of retired government workers, the indictment says. Prosecutors say that Individual A worked as a spotter and assessor for Iranian intelligence.
A few days later, Witt wrote to the same person, "I think I can slip into Russian Federation quietly if they help me and then I can contact wikileaks from there without disclosing my location".
In 2013, Witt traveled to Iran for that year's "Holywoodism" conference. Iran's nuclear program was the target of the U.S.
"I loved the work, and I am endeavoring to put the training I received to good use instead of evil", she allegedly told her IRGC contact.
She eventually did, with help from Individual A, in August 2013.
"On or about July 3, 2013, Witt wrote Individual A, 'I think I can slip into Russian Federation quietly if they help me and then I can contact WikiLeaks from there without disclosing my location", the indictment said.
Provided with housing and computer equipment by the Iranian government, Witt tracked down USA counterintelligence agents she used to work with on Facebook, the indictment said, and disclosed the classified identity of at least one of those agents, according to the charges.
During her government career, she was granted high-level security clearances and "deployed overseas to conduct classified counterintelligence missions", the DOJ said.