Ya, that PSU looks like it will work fine. It seems to have a powerful 3.3V rail as well, so you could use that and not use any resistors for your LEDs, making wiring much easier and more efficient.
The 12V rail looks powerful enough to handle a few cathodes also. YOu don't need separate rails for each cathode, but the specs said that each requires .7A, so allow for that.
Yes, a PC PSU is overkill, but it'll do the job and is easy to find, in my opinion. Since it easily handles 3A, you don't necessarily need to add circuits to make the LEDs more efficient, but that doesn't hurt. If you hook them up to the PulseVU 2X, which handles 3A, then if you have them on the dim setting, or any setting other than on, they'll be pulse width modulated, thus making them more efficient.
5Vsb is 5 Volt Standby, meaning it is always on, whether the PSU is on or not.
For wire, you'll probably want a lot of 24awg and use a strand of that for each set of 10 LEDs. Fry's is a good shop for wire and electronics parts, or I'm sure you can find some on ebay, etc.