Mixing different speeds of ram?

Assuming you are running it at the speed of the slowest memory (667 MHz), you should be fine. While the timings for the 1066 RAM are CL5, and the 667 are CL3, I would imagine that the 1066 could deal with CL3 if working at 667. Otherwise, you may have to reduce the timings slightly to deal with the lowest common denomiator.
 
It's never a good idea to mix memory type as you'll almost certainly get different memory chips on the different sticks which can cause problems.

Saying that, I've been running 2x1GB Team Xtreem and 2x1GB Crucial Ballistix for a while now at DDR2-800 and had no problems so yes it's possible.

Good idea would be to stick each pair in and do some testing to see what speeds/timings they run at, then pick the best combination and try the 4GB.
 
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