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Its Half Life for me. I think it provided the following:

It created a new way to tell stories in FPS games, traditionally it was done by loading screens prior to HL.
The open nature of the HL engine spawned multiple mods that have become massive success in their fields. HL spawned Team Fortress, Day of Defeat and Counter Strike, some of the best multiplayer experiences ever created and they laid down a lot of framework for the modern day FPS.
HL2 launched Steam, the first really successful digital Download service on PC's.
HL2 introduced the source engine which powered 5+ years of great games and it also introduced physics into the FPS world.
They moved character interaction to a new level with Alyx.
It ultimately spawned a little mod that came to be the game Portal, which once again pushed new boundaries.

The above is just off the top of my head but there is so much more that can be said and the games happened to also be great at the time too. This for me its the best/greatest/most important series of FPS games.

P.S. Massively biased as I did spend 2 years solid playing TF2 online