Trappe, 39, took off from Maine Thursday morning. He expects to make it to Europe in three to five days.
He already holds the record for the longest-ever cluster balloon flight, which lasted 14 hours and involved balloons tied to an office chair. He also was the man behind making a real-life version of the floating house in Disney-Pixar's "Up."
"This is far greater than anything achieved before," Trappe said. I'm looking at 62 hours or longer.".
He will fly wherever the wind takes him, and could end his journey anywhere between Iceland and Morocco. To control the "Up"-inspired cluster, he will pop balloons or drop ballast.
During conventional attempts -- those conducted in hot air balloons -- five people have died while trying to cross the Atlantic.
But Trappe floated on undeterred, as he took off for the 2,500-mile trip early Thursday morning in a lifeboat suspended by 370 colorful balloons.
"If I touch down on water then the attempt will be over as it will be impossible to take off again, but the boat will keep me alive," he said. "It will be incredibly dangerous as I could be several days away from any rescue crew and it will mean surviving rough seas for a long time, alone."