The Grunfeld is very sharp and theory-heavy, so if you have many many hours and a sharp memory, go for it. Otherwise, stick with the Nimzo.
nimzo-indian vs the gruenfeld

There are two volumes on the Grunfeld by Boris Avrukh which are supposed to be very good. I've ordered them for my own library, but they're still shipping and so I can't make them a specific recommendation - I suggest you go read some of the reviews out there about them first.

Problem with the Nimzo Indian though is that you will have to learn something like the Queens Indian or the Bogo Indian along with it.
I know there's nothing similar about these two openings but I enjoy playing them both but if I should put serious time into learning one of these which should it be?