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We have two dozen infant size regular Indian prefolds (unbleached). I just ordered two dozen premium size regular Indian prefolds (organic). Personally, I think organic is worth the extra cost because it means fewer chemicals and a smaller environmental impact.
I haven't tried the smart fit but am kind of curious. It seems like a good idea and I kind of wished I had ordered them this time around...
As far as bamboo, I've heard good things about it regarding absorbency and, from what I understand, it is has a lower environmental impact than cotton.
I would only get infant size if I was expecting skinny babies, and/or I was not planning to fasten them, just trifold in covers. They are much more narrow than the Smart Fit/sized style and usually cannot be fastened for long since the width gets outgrown fast. They are nice and long though so work for trifolding throughout a big size range. Some small babies potty learn out of infant prefolds but that is rare! Twins are often small so it might be a good way to go for you.
Smart Fits are shorter and much wider. If you get every size, you often can get away with not having to fold down the length at all. So you can fasten them well and don't have extra bulk from the fold down. Basically they fit better but the downside is a lot more sizes to buy. You can skip sizes though. Like many people skip newborn and medium. Then you can do great with smalls and larges and it is not much different from doing infant and premium in the traditional system. Except that they are much wider and can be fastened more easily.
I have only ever used 100% cotton prefolds. I know bamboo is popular for softness but in my experience, it is a less durable fabric than cotton. I would stick with cotton. Organic or not is up to you and your level of environmental concern and budget, it is not much difference in the final product.
^^ I think you have gotten some great advice. We have the Smart Fits, and we did order every size. The newborns were actually a little big on our teeny girl when she first came home (she was 5 pounds 14 oz when we left the hospital), and they lasted a while for us, so I don't regret it. But if you are expecting average-ish size babies, they might not be worth it.