There was no major breakthrough during the meeting, and President Trump reiterated his interest in acquiring the island shortly afterwards.
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Lars Lokke Rasmussen said the meeting with Vice-President JD Vance and Secretary of State Marco Rubio on Wednesday had been "frank but constructive". But he added that US President Trump was insisting on "conquering" Greenland which was "totally unacceptable".
"We made it very, very clear that this is not in the interest of [Denmark]," he said.
Trump afterwards reiterated his interest in acquiring the resource-rich island, a position that has rattled allies across Europe and stoked tensions with Nato.
The hour-long meeting between the US, Denmark and Greenland failed to bring a major breakthrough, although all sides agreed to set-up a high-level working group to discuss the future of the autonomous Danish territory.
Rasmussen said there were "red lines" the US could not cross, and the working group would meet in the coming weeks in an effort to find a compromise. He added that Denmark and Greenland were open to the possibility of the US opening more military bases on the island.
"It's productive to start discussions at a high level," he said.
Rasmussen also said there was an "element of truth" in Trump's view that security should be bolstered to counter Russian and Chinese interests in the Arctic. But he said the president's comments about the presence of Russian and Chinese warships around Greenland were "not true".
Watch: What message do Greenlanders want to send to Trump?Despite being a sparsely populated territory, Greenland's location between North America and the Arctic makes it well placed for early warning systems in the event of missile attacks and for monitoring vessels in the region.
Trump has repeatedly said acquiring it is vital to US national security.
The US already has more than 10