This is a good question; thank you for posting. For me it was probably the original Unreal and having a dedicated 3D graphics card for the first time to play it on. I of course had played its historical predecessors in Wolfenstein 3D and Doom and such, which also amazed me at the time. But Unreal felt like a magical leap forward.
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Ultima Underworld for me. Coming from simple 2D NES games, a 3D world populated by NPCs you could hold conversations with and items that respond to rudimentary physics was mind-blowing.
Age of Mythology for me after my first ever game of Age of Empires 2 AOK
Wolfenstein 3D
The graphics and gameplay were mind blowing at the time.
Quake was pretty mind-blowing. Full room-over-room and all.
It might have been the first far cry game or possibly doom 3, I forget what came first.
I distinctly remember "Redneck Rampage" being the first game I'd ever played with an install over 100MB and it blew me away - that felt absolutely MASSIVE at the time.
The physics engine in "Jurassic Park: Trespasser" also knocked my socks off. I wish that one would get a re-release on GOG or something; it's terrible, but I've got a lot of fond memories bumbling my away around that island.
For me I'd say it was probably playing Carmageddon 2 at my friend's place. I think that was also the first time I played a 3D-accelerated game (Voodoo).
Dungeon keeper 1. Real time strategy and first person shooter at the same time. Its like playing strategy game with a view from the top and then you can switch to Minecraft mode, dig the walls, build things, fight enemies.
The first 3d(not top down) GTA game...the freedom to explore was epic