First you need to need to pick a moderate/attainable clock speed that your happy with. Once you've decided on a target for your cpu increase the FSB, incrementally, <10Mhz (reduce this to 5Mhz when neccessary) at a time until it becomes unstable - then increase your Vcore voltage slightly and start the process again. You may need to decrease the ram divider at times as the FSB will take it over stock - and sometimes, yes, the ratio may take it below its stock running speed - but this can be sorted after you've reached your first cpu clock target.
It's imporatant that you choose a mederate/attainable clock at first just so you can get the feel of your system and the BIOS.
Once you've prime95 your new clock you can then either work on your memory settings or look again at getting a highter clock either by repeating the same process or you may want to find your max FSB in which case you will need to reduce your multiplier it's up to you. (When going for high clocks you usually always have to reduce your memroy timings just so that you take that component out of equation when trouble shooting stability issues - they can be worked on once your system is stable at clock, as already mentioned.)
Sometimes there is a trade off in memory setting when going for a high clock - you may have to run slacker timings and below it's true speed (my timings are on default but i have had to run my memory approx 200Hhz under it's true speed.) It's a personal choice, personally i prefer the larger cpu boost and a moderate under clock of my memory as i feel the difference is negligiable. (i could play around and probablt get my memoery up to speed but i can't be bothered at the mo as my system is very stable.)
All personal choice - and depends largely on what you'll be using your system for as to whether or not your happy having minor underperforming memory. Having said that you may get both working well together at the clock speed you want - even your memory may get a boost too.