The exchange came as Pompeo, President Trump’s longest-serving and closest senior adviser on national security, has been criticized for his conduct related to both Ukraine and Iran and his disregard for congressional and media questions about it.

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In a statement, Pompeo called the NPR episode “another example of how unhinged the media has become in its quest to hurt President Trump and this Administration.”

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Known for his bombast during three terms as a congressman from Kansas, Pompeo has had an increasingly rocky relationship with the news media, sometimes snapping at journalists and refusing to address questions he has labeled, among other things, “ridiculous” and “ludicrous.”

A major reason the president values Pompeo is because the secretary “doesn’t give an inch” in public statements and interviews, said a senior administration official, who spoke on the condition of anonymity to discuss internal deliberations. Pompeo rarely lets any criticism of the president or his policies go uncontested, and he is aware that Trump closely monitors his words.

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But he has grown increasingly testy as his own conduct has been questioned. Senior Foreign Service officers, in sworn impeachment testimony, and many other current and former State Department officials, have charged that Pompeo has shown little loyalty to the department he leads, and its employees, in the face of Trump’s attacks on them.

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On Friday, at the end of an interview that focused largely on Iran, Kelly asked whether Pompeo owed the former U.S. ambassador to Ukraine, Marie Yovanovitch, “an apology” for failing to defend her when the president ordered her fired last spring.

Trump’s personal lawyer Rudolph W. Giuliani and his consultant on Ukraine, Lev Parnas, told Trump that Yovanovitch had bad-mouthed him to Ukrainian officials, and that she had obstructed their efforts to push Ukraine to investigate former vice president Joe Biden and alleged Ukrainian interference in the 2016 U.S. presidential election. They have said they urged the president to get rid of her.

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During a call from the department in May, Yovanovitch was told, without explanation, to depart on the next flight out of Kyiv. Trump then denigrated her in a July telephone call with Ukrainian President Volodymyr Zelensky, saying that she was “bad news” and that “she’s going to go through some things.”

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Yovanovitch, a respected career diplomat, denied the charges against her in sworn testimony during the House impeachment inquiry. She said she was “incredulous” that her superiors decided to remove her based on “unfounded and false claims by people with clearly questionable motives,” including Giuliani’s associates in Ukraine, who could have been threatened financially by her anti-corruption efforts there. She said Pompeo’s then-deputy, John Sullivan, assured her she had done nothing wrong but said she had lost Trump’s confidence.

Former senior Pompeo adviser Michael McKinley testified that Pompeo rejected repeated internal requests to publicly come to Yovanovitch’s defense, and that he resigned his post over her treatment.

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In response to Kelly’s question about Yovanovitch, Pompeo insisted that “I agreed to come on your show today to talk about Iran,” an assertion the NPR reporter disputed, saying she had told his staff she would ask about Iran and Ukraine. When Kelly persisted with questions about Yovanovitch, Pompeo said, “I have defended every person on this team.”

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The interview then ended quickly. Pompeo, NPR reported Friday, “stood, leaned in and silently glared at Kelly for several seconds before leaving the room.”

“A few moments later,” NPR reported, “an aide asked Kelly to follow her into Pompeo’s private living room at the State Department without a recorder. The aide did not say the ensuing exchange would be off the record.” The term is widely understood to mean that the conversation cannot be reported in any way.

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On the Friday evening broadcast, Kelly said, “I was taken to the secretary’s private living room, where he was waiting and where he shouted at me for about the same amount of time as the interview itself. He was not happy to have been questioned about Ukraine.”

“He asked, ‘Do you think Americans care about Ukraine?’ He used the f-word in that sentence and many others. He asked if I could find Ukraine on a map. I said yes, and he called out for aides to bring us a map of the world with no writing. I pointed to Ukraine. He put the map away,” Kelly said.

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“He said, ‘People will hear about this,’ ” she said.

In his written statement released Saturday morning, Pompeo said, “Kelly lied to me, twice. First, last month, in setting up our interview, and then again yesterday, in agreeing to have our post-interview conversation off the record. It is shameful that this reporter chose to violate the basic rules of journalism and decency. This is another example of how unhinged the media has become in its quest to hurt President Trump and this Administration. It is no wonder that the American people distrust many in the media when they so consistently demonstrate their agenda and their absence of integrity.”

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“It is worth noting that Bangladesh is NOT Ukraine,” Pompeo wrote.

In that final sentence, Pompeo seemed to imply that Kelly, who has worked extensively overseas and has a master’s degree in European studies from Cambridge University, got her geography wrong.

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Nancy Barnes, NPR’s senior vice president for news, said in a subsequent statement that Kelly “has always conducted herself with the utmost integrity, and we stand behind this report.”

The State Department did not respond to repeated requests for clarification of Pompeo’s statement.

Democrats in Congress have charged Pompeo with failing to respond to requests for documents on Ukraine and other matters. On Friday, Rep. Eliot L. Engel (D-N.Y.), chairman of the House Foreign Affairs Committee, said the State Department had again failed to meet a deadline, this time in response to a Jan. 15 request to turn over “records related to a potential threat” to Yovanovitch’s security.

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The request referenced recently released text messages between Parnas and Robert F. Hyde, a Republican congressional candidate, implying that Yovanovitch was under surveillance in Kyiv. Engel had asked for a response by Thursday.

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In a letter to Pompeo on Saturday, Sen. Robert Menendez of New Jersey, the top Democrat on the Senate Foreign Relations Committee, and four other senior Democratic senators excoriated the secretary for his NPR statement.

“At a time when journalists around the world are being jailed for their reporting . . . your insulting and contemptuous comments are beneath the office of the Secretary of State,” they wrote. “Instead of calling journalists ‘liars’ and insulting their intelligence when they ask you hard questions you would rather not answer, your oath of office places on you a duty and obligation to engage respectfully and transparently.”