what does it matter? A flight from NYC to either will cost roughly the same. You can catch a good deal (online) if you're lucky and keep looking. Otherwise one-way is gonna cost you more than round-trip.
Phoenix, Arizona is real neat for cultural studies (Spanish - Native American intermixing from 400 years ago), and has Saguaro cacti in their native habitat. (And lotsa other stuff.)
Santa Fe, New Mexico is an interesting, "counter-culture-y" place.
The Grand Canyon is pretty spectacular but I don't know if a bus will get you there.
Hit New Orleans at Mardi Gras time (late March?) for a major party environment.
Surely you want to hit Boston? It is the Hub of the Universe, after all. And you could take America's only halfway-viable train service back to NYC, if you've had your fill of Greyhound by then.
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