Treasure Adventure Game is quite good, though it was essentially abandoned by the dev after v.1.0 when he began work on its expanded commercial remake,
Treasure Adventure World, so it is a little buggy in places. But you can't beat the price!
Tannath: [...] On the other hand, Flight of the Amazon Queen is also quite good.
Seconded. Cheesy humor and a zany B-movie plot, yet it still manages to somehow be charming rather than grating.
Warsow also seems like it would be pretty cool for those into
Quake III-style multiplayer "twitch" shooters...assuming you can find anyone to play with. (I've not played it, so I can't really opine too much.) One issue, though, is that the version on GOG is apparently kind of old now, so the best place to get this game would probably be from the developers' site (it's an open-source game, I believe, so it's free there, and probably anywhere else it's hosted, as well).
As to the rest of the permanent freebies here, one's enjoyment would probably depend on whether or not one has previously played any of them, what game genre(s) one is most interested in, and how well one can stand the older graphics, interfaces, etc.