This is hard to choose for myself. I don't think I can decide on one, so I'll stick with two (three technically.)
First up is Portal. Both games. I love the creativity and style. The fact that you could make a game with one protagonist and antagonist is very intriguing to me, even more so when I think about how there is only dialogue written for one! I personally thing the second game is better than the first, which is rare for me. I love how you get to actually see GLaDOS as more of a person and Wheatley was an awesome companion. Cave Johnson was also a pleasant surprise. Overall, the Portal series (as small as it was) will always be one of my favorite playthroughs.
Secondly, I can't not mention The Last of Us. This is one of the most creative and well-written videogames I have ever played. I loved how the player is highly encouraged to do more than "spray 'n pray" through the story. The hunt for supplies and ammo was challenging and fun. The story itself was very emotional and the cast was fantastic. I don't recall a game with a better voice-over.
Honorable mentions: The Elder Scrolls V: Skyrim, Kingdom Hearts, Super Smash Bros.