Besides those old classics from the 90s and some relatively recent releases, most of the really popular ones from the past few years have already been covered. kj's wishlist above contains pretty much all the big ones left.
There are some games that deserves to be animated as well, but their length makes it difficult (Key's Planetarian, Stage Nana's narcissu, etc.).
Personally, I think a Touhou-series anime would be the most awesome thing ever.
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