Your computer will not run faster with pc100 or pc133 memory. You might compare this to putting high performance tires on a car. They don't make it go faster. They give it the ability to go faster, if it could, but they don't actually make it go faster.
Now, as far as you buying ram, you'd probably be best off buying pc66 ram
if it's available and affordable. However almost all ram of this type is backwards compatible (pretty much). You can fairly safely assume that pc100 ram will work fine in a 66mhz bus. Supposedly, pc133 will also work at 66mhz, but I've seen a number of situations where that didn't happen. So don't count on pc133 working for ya.
Considering how quickly hardware grows out of date in the computer industry, you might very well find that pc100 ram is more easily available and even cheaper than pc66 ram. If that's the case, I'd go for the pc100 without hesitation.
Any ram you put into your machine (be it pc66, pc100, or pc133) will all run at the bus speed of 66mhz.
If your motherboard has the option of setting the bus speed to 75mhz or more, then you might definitely want to get ram that's rated for speeds higher than 66mhz, this way you would have a better chance of achieving successful overclocking, if that's something you're willing to do.
Also, check to see if your motherboard uses ram that is 5volts or 3.3volts. Most likely it's 3.3v, but there were some motherboards of that 66mhz bus era that needed 5v ram. 5v and 3.3v ram are not interchangeable.
If I've forgotten anything important than I'm sure someone else will be along any minute to help fill you in. Don't go on my message alone...it's been quite a long time since I've been on a 66mhz bus.