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...any suggestions on what might be a good 'medium' to work with?

I'm thinking of mostly sculpting 28" scale... mostly because that's what I play.

is 'Green Stuff' the way to go? or is there a better material to work with?

I'm thinking for now will start with existing bits/models... and then work with them in conjunction with green stuff.

Eventually, though I'm looking to make whole sculpts.

I'm thinking about doing this mostly because I want to make my own 'Sisters of Battle' Army... or even just some generic military unit made with female looking models... I heard new GW 'sisters' might be on the way? But I'm kind of skeptical as to how those turn out.

Green stuff can be rough to work with at first. It's somewhat rubbery and also dries somewhat quickly. When I first started, I used sculpley, as it has to be baked to dry and is very cheap for a very large amount. There's ups and downs to every medium, though. Since you're looking to modify existing models, green stuff might be what you're looking for, maybe mixed with some milliput to give it better texture. You don't want to bake plastic parts :/

I do a lot of my own sculpting for the same exact reason. I play Sisters, and the model range is very limited. I work in Greenstuff because I am familiar with it. Milliput has more graduation in how it is sold, so you might do some research there. There are way better sculptors than me here, but I recommend you follow your path and use bits to start, with greenstuff work in between to get a feel for how it works. One big jump I found was escaping metal tools to sculpt with (not completely of course). I purchased a set of sculpting tools on ebay that were sillicon rubber (I believe they said they were for clay) and it has made a HUGE difference. Greenstuff sticks to metal badly, it rarely does to the sillicon. You can find some of my stuff here (my gallery) just to see if it inspires you, or at this, my webpage.
http://edwardmystcreations.weebly.com/
You'll find my sister's army is a work of love despite their really old codex...Also, look at my Imperial guard army, I sculpted a lot of females for it (and of course my sister's of steel is an all female IG army)
I still struggle with faces and such, but I grow better as I go, so will you. I really hope you give it a go, and share with us. I was mediocre at best when I started, and the people here really threw a lot of encouragement. Please ask me any questions, I will do my best to help (and if I can't, there are people here who can).

PS: I ate in a mess hall for a portion of my life...but I won't hold it against you

The silicon tools are often found labeled as clay shapers. And they are indeed awesome. Otherwise you need to keep your metal tools wet or covered in something water based like KY jelly.

I do most of my conversion sculpting with a mix of Greenstuff and Milliput, either the standard yellow grey Milliput or the superfine white Milliput, depending on what I'm doing with it. I find, as you said, that greenstuff tends to be rubbery when it dries. Milliput dries rock-solid which makes carving and sanding it much easier, but I'm not fond of how it's kind of crumbly to work with, and goes slick like clay with the addition of water.

So mixing GS and Milliput gives me the best of both worlds - it works like GS, which is much more to my liking, and dries solid like Milliput.

As for tools, so far the only things I've really used are a pin, a spare crochet needle I got from my mum, and the back of my fingernail. XD Oh and then a knife and sandpaper for shaping and smoothing after stuff's dry. Clay shapers probably would make things easier, but they're not entirely necessary.

Medium? Green stuff, maybe with milliput added to taste.

Do you go to Gencon? I took some excellent sculpting classes at one that were taught by professional sculptors. I highly recommend them.

Thanks for the input! Sorry for the delayed reply... on a California trip at the moment.

The classes at Gencon are something I definitely been wanting to check out.

My work with green stuff is limited to maybe cleaning gaps ... very little sculpting... like making grenades or fixing missing fingers or hands when I modify things.

I was just wondering if maybe some folks might be using alternatives to green stuff.

From what I understand the French use super sculpty. It's a whole different process.