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I'd say try Half Life or one of the three Quake games. The downloadable modifications for these games are extensive (and mostly free), so you'll have a hard time becoming bored. Team-based games like Team Fortress, Counter Strike, and Urban Terror provide a more structured form of play than the traditional "deathmatch" mode. If you're interested in an only slightly modified gameplay, I'd suggest modifications like Rocket Arena or OSP for Quake 3. Single player mode seems to have long lost it's allure in FPS gaming, so I don't know what to tell you if you're strictly looking for something story-driven like MGS3.
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