Not an expert, but:
Gundam
Hugely varied types of soundtracks across a sprawling series, representing many different composers. I think it would be very difficult to recommend one or even several that give an idea for the franchise as a whole. Maybe there's a certain era of the series you are more interested in?
Ghost in the Shell
Speaking only for the original movies and SAC, both are very different. You've got Kenji Kawai's moody atmospheric stuff from the films, and Yoko Kanno's gargantuan masterwork that is the SAC series. Because SAC spans like seven discs worth of music, I would direct you to either OST#1 as a really good mood-setter for what SAC is and Kanno's treatment of it, or OST#3 for some of the most amazingly imaginative and memorable anime music you'll ever hear (not hyperbole).
As a side note, a full listen of all SAC soundtracks roughly in order is an incredible experience. To be honest I wouldn't recommend that anyone "ruin" it with a best of or compilation or anything like that. I can pretty much guarantee you'll love them.
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