The Obligatory Link: Should Maryland Sidestep Electoral College?
The quick answer to that question? Not if they ever want to see a presidential candidate outside of their primary week ever again. Though, with how early everyone seems to want to get started this time around, they'll probably still be sick of it by the time the election happens anyway. There seems to be the thought, though, that this would bring candidates back to states outside of the "battlegrounds". Trick is, though, they go to those battleground states because that's where the outcome is actually in doubt. States that trend steadily one way or another are generally known quantities, and thus would be harder to shift (even for popular vote numbers), even if the candidates did put in more appearances. In other words, a time-versus-money kind of thing.
Really, the whole of this is that people are natural tamperers. To mesh a couple of old sayings together, even though the mousetrap ain't broke, they want to try to build a "better" one. All it would do is scale up the numbers involved and make any potential recount even longer and more arduous. (Think about that idea for a second: A national recount. That's scary, innit?)