I personally think that Insecticide - Part 1 deserves a place in there. It wasn't exactly polished, and yes, there was quite a small array of enemies, but the game (well, half-game) was very enjoyable. It had good voice-acting, unique and likable characters, and a really awesome atmosphere which really reminded me of Grim Fandango at times. It's so sad that there was never a Part 2 released on the PC. It would have been so nice to see the story concluded, rather than be left with a cliffhanger...
Ghost Pirates of Vooju Island would also be a nice addition to the bundle, if there were to be a second one (second bundle that is, not second GPoVI).
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Read that instead ^.
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