Special envoy Steve Witkoff flagged that the US will now consider alternative options to bring Israeli hostages home.
"While the mediators have made a great effort, Hamas does not appear to be coordinated or acting in good faith," Witkoff said.
He said it was "a shame that Hamas has acted in this selfish way" and that the US is "resolute" in seeking an end to the conflict in Gaza.
Hamas said it was surprised by Witkoff's remarks, adding that the group's position had been welcomed by mediators and had opened the door to reaching a comprehensive agreement.
"The movement affirms its keenness to continue negotiations and engage in them in a manner that helps overcome obstacles and leads to a permanent ceasefire agreement," Hamas added in a statement early on Friday.
A breakthrough in talks on a ceasefire deal between Israel and Hamas has eluded the Trump administration for months as conditions worsen in Gaza.
The territory recently had its deadliest day yet for aid-seekers in over 21 months of war, with at least 85 Palestinians killed while trying to reach food on Sunday.
Dozens of people have starved to death in recent weeks in Gaza.
The sides have held weeks of talks in Qatar, reporting small signs of progress but no major breakthroughs.
Officials have said a main sticking point is the redeployment of Israeli troops after any ceasefire takes place.
Earlier Thursday, Israeli Prime Minster Benjamin Netanyahu's office recalled his country's negotiating team back to Israel in light of Hamas' response.
In a brief statement, the prime minister's office expressed its appreciation for the efforts of Witkoff and mediators Qatar and Egypt, but it gave no further details.
The deal under discussion is expected to include a 60-day ceasefire in which Hamas would release 10 living hostages and the remains of 18 others in phases in exchange for Palestinians imprisoned by Israel.
Aid supplies would be ramped up and the two sides would hold negotiations on a lasting truce.
The talks have been bogged down over competing demands for ending the war.
Hamas says it will only release all hostages in exchange for a full Israeli withdrawal and end to the war.
Israel says it will not agree to end the war until Hamas gives up power and disarms, a condition the militant group rejects.
The State Department said earlier in the week that Witkoff would be travelling to the Middle East for talks, but US officials later said that Witkoff would instead travel to Europe.
It was unclear if he was holding meetings there on Thursday.
Trump earlier this month met Netanyahu at the White House, putting his weight behind a push to reach a breakthrough and a ceasefire agreement.
But despite his newly strengthened partnership with Netanyahu following their countries' joint strikes on Iran, the Israeli leader left Washington without any announced breakthrough.
