"Regarding registration and sharing (of refugees), European cooperation and solidarity have completely failed," he told the Frankfurter Allgemeine Zeitung (FAZ), cited in German in the paper's Friday print edition.
The Italian, who took up the UN job on January 1, also warned against European countries closing their borders which would de-facto block many refugees, already in distress, in Greece.
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"Our message aimed at Europe is: 'Pull yourself together,' and 'deal with (the situation) yourselves'. But if our help is needed, we will be there."
Grandi notably pointed the finger at an EU deal struck last summer on sharing out some 160,000 refugees, and which has gone nowhere ever since. Only 583 "relocations" have actually gone ahead due to foot-dragging by certain countries, notably in the continent's east.
"Yes it is important that the system (of sharing) be applied, but it will be difficult," said the UN official. "At the moment, I don't see a lot of momentum in that direction."
According to UNHCR figures, more than a million migrants arrived in Europe by sea last year.
Non-governmental organisations (NGOs) have repeatedly condemned what they see as indifference by EU member states towards the fate of those fleeing war and misery.
While most of her EU colleagues have turned their backs, German Chancellor Angela Merkel has proved "courageous," said Grandi.
Germany opened its doors to over a million asylum seekers in 2015. Despite criticism from part of her governing coalition, and growing unpopularity among ordinary Germans, she has refused to set a ceiling on numbers for this year.
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