Well, for the most part, the most important settings in a game include texture details, anti-aliasing and anisotropic filtering. The first thing you want to do when loading up a game is to change the resolution to the maximum that your monitor will support. From there, crank all of the settings up to max, and then work from there. If the game doesn't run well with "Ultra" texture detail, for example, decrease it to "High" and try again.
If you think the card is up to the task, then start raising the anti-aliasing. 4x is probably going to be the max for most games on that card. The resolution matters too. If you are playing on a 20" monitor or lower, you could probably max out the settings for any game out there no problem (save for Crysis). At 24", most games should still run great, but at max detail settings, anti-aliasing might be a problem.
Just experiment. Crank the settings to max and then work your way down to see what works the best. It will be different for each game title.
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