Bus speed overclockability is dependent on many variables. Your PCI cards have to be able to handle an increased bus speed, so does your memory, so do your IDE controller , chipset and hard drives and CDROMs.
Increasing the speed of the CPU only depends on the CPU being able to handle the increased speed, which almost all newly purchased CPU's can do because both AMD and Intel have very good quality control as well as very good fabbing methods these days. They're producing a lot of chips which they COULD mark as much higher speeds, but they have to supply a certain number of the lower speed chips to meet the demand. So what could have been a 900MHz CPU gets marked as a 600MHz (after testing that it CAN do 600MHz) and they don't bother to check whether it will go higher. So you buy it for the price of 600MHz and find out that it CAN do 900MHz, and you get a free 300MHz.
Overclocking the bus does provide a lot of performance gain, which is why people were doing it before Intel multiplier locked their CPU's. Now that they can't just change the multiplier, it's the ONLY way to overclock an Intel. (Athlon/Duron/TBird require some work to do it, but you can still change the multiplier on them.)
Overall, the CPU speed is far more likely to be overclockable by a wide margin than the bus speed is going to be able to. You might have an Intel CPU capable of being overclocked by 300MHz, but the FSB on your motherboard may only be able to go up to 112 or something due to a picky IDE controller or hard drive, or your AGP card may not like the non-spec AGP speed. With a marked-as 550 PIII (100MHz bus), that's only a 66MHz increase in speed for the CPU. So you're pretty much stuck with that.
If you've got an unlocked CPU, like a modified Duron, you could increase the bus speed to 112 AND increase the multiplier, giving you even more performance increase.