each drive will run at the it's highest spped possible, as long as the motherboard supports it. Currently your computer will run all drives at ata66. The effect is that when transferring certain types of data, transferring at 133, a 5400rpm drive can lag, thus the faster spinning drive of 7200rpm.
As for the upgrade theoretically it could speed up your device, but data still can only move as fast on the motherboard as there are physical wires, which in your case is 66, not 133. To get proper performance from your computer a new motherboard sounds like the real upgrade. What kind of processor do you have?
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