Just about everyone in this thread has given my best picks. My favorite story in any game this generation is probably Red Dead Redemption, but sadly its not on PC (though definitely check it out if you are ok with a slow start). Here are my picks:
Portal series
Grand Theft Auto series (the earlier ones had fun gangster tales, but IV dropped the ball in amazing writing)
Bioshock (pretty much impossible to miss this one)
Half-Life series (the stories themselves aren't too shockingly new, but the presentation and writing goes a long way, plus apparently Quentin Tarantino loves the Half-Life series so take that to heart)
Mass Effect series (just play it, and you will see because I don't even want to spoil anything about this amazing series)
Max Payne series (the gameplay is a tad dated, but the series just drips with dark noir, and its a good way to get caught up before Max Payne 3)
Alpha Protocol (the story feels familiar, but the writing is top notch, and Obsidian definitely knows how to craft a good tale)
Fallout series (pretty much everyone of these games has a great tale I'd say, but the older ones are incredibly slow paced so you might want to start with 3 and New Vegas if you don't like turn based combat)
Deus Ex series (mainly Human Revolution and the first game, I've only tried a bit of the second so I wouldn't know about it too well)
Batman: Arkham Asylum/City (my avatar and quote made this something I HAD to include, but if you like comics or heroes even a tiny bit, then check these amazing games out)
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