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Raonic came to Flushing Meadows with high hopes, instead the Canadian star suffered a shock 6-7 (4-7) 7-5 7-5 6-1 defeat after three hours, 37 minutes on Wednesday.
Buoyed by his semi-final run at the Western and Southern Open, Raonic looked good early in warm New York conditions as he claimed the opening set in a tie-break.
Raonic seemed to slowly tire from that point in New York, the 25-year-old thwarted by Harrison, who saved nine of 10 break points in a 70-minute second set.
The third was a difficult one with Raonic calling a medical timeout for his wrist during another marathon set, which saw his service percentage drop to 38.
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It got worse for the deflated-looking Raonic in the fourth, which proved to be his final set, as Harrison served out the match to love.