Way I do it is up the FSB a bit at a time, then up the voltage until it doesn't boot or freezes. Once I'm happy with the speed I'll do some stress testing to make sure the temperatures are good, sometimes needs a bit more voltage to keep it stable.
There's a lot more to it than that to get it spot on, but it's how I start off! My Q6600 will sit at 3.6GHz nicely. I'm currently at 3.2GHz due to folding 24/7 though
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