Education Secretary Linda McMahon sent a three-page letter to Harvard President Alan M. Garber blasting the school for "disastrous mismanagement."
“This letter is to inform you that Harvard should no longer seek grants from the federal government, since none will be provided," McMahon wrote.
Tensions have risen between the Trump administration and elite universities over issues including admissions, hiring practices, curriculum oversight and responses to pro-Palestine campus protests.
The Trump administration has already frozen more than $2.2 billion in federal grants to Harvard and $60 million in contracts.
Harvard has sued the administration in response, alleging that the funding freeze violates the First Amendment and federal law, which bars the president from directly or indirectly ordering the Internal Revenue Service (IRS) to conduct or terminate an audit or investigation.
"In every way, Harvard has failed to abide by its legal obligations, its ethical and fiduciary duties, its transparency responsibilities, and any semblance of academic rigor," McMahon said.
She added that the administration had previously been willing to maintain federal funding to Harvard as long as it committed to complying with federal law.
"At its best, a university should fulfill the highest ideals of our nation and enlighten the thousands of hopeful students who walk through its magnificent gates. But Harvard has betrayed its ideal," she said.
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