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low rated
I want more lego games, you can post the series that you want more games on gog!
More Crysis games!
More Star Wars rpgs like Kotor, but in a different era
More Psygnosis (developed, published or ported) games!
Star Trek.

Although technically speaking they are not from the same series, as they are based on different TV series, and developed by different companies.
Silent Hill and Shenmue.

Also, not a series, but I'd really want to see the rest of the Cinemaware games here, especially It Came from the Desert.
Mainline Dragon's Dogma games...

... and...

... Castlevania games
Splinter Cell
Dead Space.
More Resident Evil games. Currently GOG sells none of them - I'd like there to be more.
Castlevania, Silent Hill, Metal Gear (at least MG2), R-Type (most of those aren't on PC, so that's definitely wishful thinking), Wonderboy, the rest of the Wolfenstein and Doom games, the first five Wizardry games.
Mortal Kombat please!
Lego is a very good call. Castlevania and Metal Gear would be my next picks as well. I'm also very interested in seeing more Street Fighter, Double Dragon, Splinter Cell and Assassin's Creed here.
Serious Sam
Worms
Unreal Tournament (missing 2003)
Dead Space
Dragon Age
I wish there were more Assassin's Creed games on GOG. It'd be great to be able to buy them DRM-free.