Meeting with US Secretary of State John Kerry at the State Department, coalition president Khaled Khoja thanked the United States for giving more than USD 3 billion in aid to the Syrian people since the outbreak of the war in 2011.
Speaking through a translator, he said he would brief Kerry on the latest political and military developments.
"We are here also to ask the assistance of the US in establishing safe havens in liberated areas."
Successive attempts at launching peace talks have so far proved fruitless.
A key sticking point has remained Assad's future, with the National Coalition insisting he must step down, a demand refused by the government.
"President Assad has no legitimacy and he's not a part of the future of Syria and for that reason he needs to be prosecuted ... For the crimes he has committed against the Syrian people," Khoja insisted.
A delegation from the National Coalition will attend discussions in Geneva on Monday, when UN envoy to Syria Staffan de Mistura is to hold separate talks with the rival sides.
Assad's regime "has lost all sense of any kind of responsibility," the top US diplomat said, adding there must be a transition "towards a government that represents all of the people and can repair this extraordinary damage."
Assad was "busy destroying the country in his own interests," Kerry said, adding that the Syrian leader was "enabling and attracting terrorists" such as the Islamic State which has seized control of a part of the country.
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