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Yes, there are a good few games to which GOG has introduced me that I've very much enjoyed. Note that this is by far an incomplete list. With my never-really-dwindling backlog I'm sure there are a number of games in my GOG library that may need to be added to the following:

Startopia
King of Dragon Pass
Original War
Fallout
Locomotion
RollerCoaster Tycoon
Stonekeep
Mostly I just buy games I've had in the past, but for your question I'd have to say Two Worlds - which isn't "old" in the sense of a lot of other games here, but I probably wouldn't have gotten it otherwise.
The one that jumps to mind for me is NOX. I hadn't really heard much about it before it showed up here and I really enjoyed it .
Jagged Alliance
Divine Divinity
Master of Magic

are incredible games I would never have tried out if it wasn't for GOG.
Definitely Gothic 1 & 2, Arcanum and Arx Fatalis for me.
Also got me back into Neverwinter Nights.
Let's see

Outcast
Septerra Core
Anachronox
NOX
Planescape:Torment
MDK
Sacrifice
King of Dragon Pass(well that was more like a re-introduction, played it ages ago and forgot about it)
Betrayal at Krondor
Theme Hospital
Starflight 1+2
Arcanum
Gorky 17
Giants: Citzen Kubto
Startopia
The Tex Murphy series
Simon the Sorcerer
Realms of the Haunting
Blood
Syndicate
Magic Carpet
Soulbringer(hey I liked it)
Lands of Lore 1
Yup. Most of the games I own on GOG were first-time titles, as a matter of fact. Baldur's Gate 2, Planescape, Outcast (which I really need to reinstall), Ultima Underworld, Arx Fatalis, Blood, Rise of the Triad, and Beneath a Steel Sky are a few that come to mind.
I buy most old games on GOG that I already played before but I think the title that comes to mind is Legacy of Kain series as I had never tried it before, I also have King of Dragon Pass in my backlog which I never heard about before GOG
Giants: Citizen Kabuto and Outcast. I must have seen them in magazines at the time but I have absolutely no memory of them. Many thanks to GOG and her community for introducing me to these fantastic games.
-Arcanum
-Fallout
-King of Dragon Pass
-The Longest Journey
-SMAC
-Planescape: Torment
-Deus Ex (well I'd heard of it before, obviously, but never played it)
-Sanitarium
-Tex Murphy
-Still Life
-The Last Express
-Ultima Underworld
-Zeus + Poseidon
-Total Annihilation
-Master of Magic

I'm a youngun' so most of the games on GOG are new discoveries.
I'm only 13 years old. First non-shovelware game I can remember playing was World of Warcraft. Does that make you feel old?

Might & Magic III - VI: I always was a huge fan of HoMM III but I didn't know what to expect. Wow, they are fantastic games. Combat is mediocre but everything else more than makes up for it.

Thief II - After three games people claimed were awesome but I hated (Deus Ex, Morrowind, SMAC), I was very nervous about Thief II. Just to make it worse, I am very impatient and HATE old stealth games. Thief II surprised me. I was having a ton of fun, because the game gives you options and understands YOU ARE NOT STUPID, without becoming the extremely frustrating "One pixel out of cover and you get bullshit detected" nonsense. Also I enjoyed getting lost in the level and picking up everything, and then reading the notes. And the story is fantastic. It's not sunshines, lollipops, rainbows, and a superhero main character. NO. This is a dark and gritty story and Garrett is just a man trying to steal, not save everyone. Wow.

Fallout - I got this for free, and I wasn't expecting much because most people who LOVE Fallout 1 HATE Fallout 3/NV. I liked Fallout 3 because of the atmosphere (NV did better gameplay). The atmosphere here is even better, the jokes are great, and the gameplay isn't too bad either.

Baldur's Gate II - My dad played this in university a bit too much (Never beat it though), and everything he says about the game made me purchase it. I never thought I could be so immersed into a game's story. It's just so great. The gameplay feels a bit odd though, and it gets annoying being attacked by murderers every 30 steps in the city. I play it about once every 1-2 weeks.
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Overrwatcher: I'm only 13 years old. First non-shovelware game I can remember playing was World of Warcraft. Does that make you feel old?
Dude... I'm 21 and you make ME feel old :P
GOG is good because it reminds me about all the titles I used/wanted to play back in the day and forgotten about them by now.
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Overrwatcher: I'm only 13 years old. First non-shovelware game I can remember playing was World of Warcraft. Does that make you feel old?
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Licurg: Dude... I'm 21 and you make ME feel old :P
I'm 17 and it makes me feel old. :/
i'm 27. thought i'd join in the age naming fun.

anyways: here they are, my gog cherry's:


nox
arx fatalis
lands of lore 1 and 2
simon the sorcerer
ultima underworld
ishar
fallout
arcanum
lionheart
septerra core.