I'd definitely go for Syberia pack. The puzzles are moderately difficult, there are lots of beautiful cutscenes and the storyline just pulls you into that world. The environment and the characters are very detailed and as it was said before, that kind of game looks good even years later.
It's not on the list, but Still Life would be a good choice too. Now that it has a sequel coming up, it would be a good time to (re)play that one.
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