Maybe you arent understanding what people are trying to say or maybe I am not understanding you. Lowering the CPU multiplier and the RAM speed (100,133,166,200) while maxing out your FSB tells you what is the MAX FSB your mobo will support. Lets say it's 278mhz.
Then you run your RAM speed at a 1 to 1 ratio with your FSB and it will tell you what your MAX RAM speed is. Lets say it's 242mhz.
Then you restore your stock CPU setting to whatever it is (lets say it is 10) and you get 2.42Ghz. If it is not stable then you would have to either lower the mutiplier or up the voltage. Am I right CHIPDEATH?
If we take your question at face value (meaning either method results in the same clockspeed), then no, it will not always yield the best results. Why? If you run your RAM at super high clock speeds to match your FSB, you will most likely have to loosen your timings and your command rate. You may find you have fast RAM that just doesnt perform better than slower RAM with better timings.
If you are trying to encode video, I would take higher speeds over tighter RAM timings. If you are gaming then go for super tight timing. But that is just my opinion. Others will most likely take tighter timings no matter what I imagine.