I already have VTMB and it works fine in Vista(not sure about 7) but I still wouldn't mind having another source for that game in case the discs go bad/missing. Arcanum and TOEE are must haves for GOG. I would be willing to bet they would have to get more servers as the amount of downloads would bring the site down XD.
I would like to see the entire Infinity Engine collection on here.
Anything Looking Glass would give GOG /. access to my wallet.
The GoldBox series from SSI is another wallet-opener for me. I miss the purity of the old D&D rules before all the convoluted min/maxing and builds came in to sort of spoil the D&D universe for me.
Darklands and The Legacy:Realm of Terorr because I want to play those in fullscreen without color hallucinations and I just want a 100% legal copy of those games since I don't like abandoneering.
apexultima: Everything made by Psygnosis :P
Its an endless list of awesomeness :D
Lemmings
Wipeout
Sentinel Returns
Blue Ice
Pyrotechnica
Endless i tell you!!!!
But it is a shame that Walker was a amiga only release :(
What about the Ecstatica games??