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If you're in the market for organic, vegetarian, and the like, Earth Fare's a great place.
My wife and I are starting to enjoy eating at the deli for quick food, about as expensive as a fast-food place but much more interesting variety.
The groceries are how one would stereotype an organic/vegetarian shop: over-priced. But if you need something special (like cardamom pods) it might the only place in Charleston you can find it. Plus they have bulk bins for some things that puts them at a good prices (like red lentils or bulgur). If you really like organic produce, you probably won't mind the extra price. They have an extensive wine and fine cheese selection. If you're looking for ingredients for a certain cuisine, in particular various Asian recipes, then it's a great place to find it.