A bus might make more sense on a shorter trip (like the aforementioned NYC to Boston example), but I think there's a real sweet spot for taking the Amtrak on trips longer than, say, 4-5 hours on the bus but shorter than a 2 hour flight (excluding baggage/security/travel to and from airport time).
Especially Amtrak's business class, which is extremely comfortable, with plenty of space for a computer and stretching out, quiet and spacious enough to get work done, and usually only an extra $20 or so.
I admit my fear of flying sways me toward Amtrak when a flight might make the most sense, but to me a bus is almost always the worst possible transportation option available.