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Anything Lucas Arts.
There are tons of games I've missed over the years, but nothing springs to mind as an 'insta-buy' for me except possibly the Homeworld games. I've never played them, but I've read such good things across numerous different forums and review sites, that I think I'd probably grab them on day 1 if they ever showed up here.
Post edited January 17, 2012 by Coelocanth
Mechwarrior (anything), X-com, and Hero X.
I don't usually "insta-buy" games. The only ones I would buy instantly if they came to GOG are Road Rash and Test Drive 5. When I got my first computer I couldn't wait to play these games when I got home from school.
Oh, and I suppose if GOG ever got Chasm: The Rift or Vivisector: Beast Inside (which they never will), I'd buy them instantly, and probably hold a few giveaways to boot.
Wizardry 8
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Neobr10: 1) System SHock 2
2) System Shock 2
3) System Shock 2
4) System Shock 2
5) System Shock 2
This, except for the random capitalised H.
Age of Empires 2
Star Trek Elite Force 1 & 2
NOLF 1 & 2 (even though I own the disks)
Populous The Beginning
Black & White 1 & 2'
Battlezone II
Rollcage
Re-Volt

A number of titles might just be bought as gifts, too, just to share the love I have for those games!
Post edited January 17, 2012 by csmith
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overread: That game with the shark gun by the people that made Kabuto - I've totally forgotten its name - but that game just because its more of the Kabuto crazy madess kind.
Armed and Dangerous. Great game.

My insta-buys -
No One Lives Forever 1 + 2 (I already own the discs as well. They really are that good.)
Aliens versus Predator 2
System Shock 1 + 2
Lemmings
Omikron: The Nomad Soul
Sid Meier's Gettysburg! + Antietam!
Beavis and Butt-head in Virtual Stupidity
Birthright: The Gorgon's Alliance
Sid Meier's Pirates
Dark Sun
I know I'm missing a few but I can't think of them right now. Once somebody else mentions them I'll probably say "oh yeah that too".
anyhoo:

Day of the Tentacle
Grim Fandango
System Shock 2
NOLF 1&2
Clive Barker's Undying
Grim Fandango
Full Throttle
X-Wing vs Tie Fighter
Star Trek Elite Force 1 & 2
No One Lives Forever 1 & 2
Age of Empires II
Ultima VIII
Ultima IX
Clive Barker's Undying

There is probably more I am not thinking of but those came to mind just now. Of all of them I most especially am hoping to see the final two installments in the Ultima series so I have them all. I'd really, really love replaying Undying again too. That was such a great game.

OMG! I almost forgot, System Shock 1 & 2!
Post edited January 18, 2012 by dirtyharry50
Being out of a job very soon, I don't have "instabuy" GOG games at the moment considering I already own them on floppy or CD ... except for those rare games that refuse to run on Windows 7. Star Trek Generations, for example.
Albion
Thief series
The Settlers 3 and 4
Battlefield 2142 Deluxe
Full Throttle
HALO 1
HALO 2
Homeworld I
Homeworld I: Cataclysm
Homeworld II

Quake Wars: Enemy Territory
Star Wars: Tie Fighter
Star Wars: X-Wing
Star Wars: X-Wing- B-Wing
Star Wars: X-Wing Alliance

Tom Clancy's Ghost Recon: Gold
Tom Clancy's Rainbow Six: Gold
Tom Clancy's Rainbow Six: Rogue Spear
Tom Clancy's Rainbow Six: Rogue Spear- Black Thorn
Tom Clancy's Splinter Cell II: Pandora Tomorrow (still works on XP)
Unreal Tournament 2003

@Red_Avatar

Have you tested your floppies and CDs since first buying them? I would advise backing them up to an external harddrive as image files if possible.
Post edited January 18, 2012 by u2jedi