Filippo Grandi from the United Nations High Commissioner for Refugees (UNHCR) said on Tuesday that he would ask all countries to step forward and agree to take another 400,000 Syrian refugees.
Grandi underlined that the world must do more to end the Syrian crisis during his first visit to Washington since being appointed as head of the UN refugee effort.
"On March 30, I'm going to chair a meeting in Geneva at which I ask the international community to take 10 percent of all the Syrian refugees," Grandi said.
"Ten percent is a lot of people. It's more than 400,000 people," he told reporters, on the fifth anniversary of Syria's bloody civil war.
More than four million Syrians have fled the conflict-torn country since the crisis erupted and more than six million are displaced within its borders.
Neighbouring Turkey, Lebanon and Jordan are struggling to deal with the influx of refugees and ongoing mass immigration has created a political and humanitarian crisis in Europe.
Some countries, including the United States, have been criticised for not welcoming refugees as Canada and Germany are stepping up their efforts to shelter them.
The US has struggled to offer new homes to desperate Syrians amid an atmosphere in the run up to November’s presidential election.
US President Barack Obama ordered that 10,000 refugees be admitted during the 2016 fiscal year, but half-way through the period only 1,115 have been processed.
Grandi lamented the tone of the debate in both the US and Europe, where anti-immigration politicians have claimed that terrorists allegedly hide among refugees.
Grandi also complained on a visit to the European parliament that he heard "language we haven't heard since the 30s" from opponents of resettlement.
However, Grandi added that the new 400,000 target figure could be met in part by means short of the full resettlement package that the US offer.
"We're really observing one of the worst political failures in modern history," Grandi complained.
"The failure of the parties to the conflict. The failure of the regional powers. The failure of the global powers to get them to come to an agreement,” he said.
"In the absence of that -- and we have to be hopeful -- it is important to show solidarity in every possible way."
Some countries may offer temporary jobs, scholarships or humanitarian visas rather than providing Syrian refugees with new lives and permanent residence, he said adding that his office would work with private firms and universities in partnership with states to try to reduce the pressure on Syria’s neighbours.