I have a dual-boot system, Windows XP32 and Vista64, with 6Gb of RAM and a 1Gb EAH3870X2 graphics card.
On XP, by the time the OS has nicked 512kb of RAM and the graphics card has pinched 1Gb to ghost, the sim has about 1.5Gb of RAM left to play with. In Vista, the OS takes 1Gb (b***y Vista), the graphics card takes 1Gb, but the sim has 4Gb to play with. Needless to say, it runs a lot more smoothly and although the frame rate is no higher, it has a tendency to stick at the lock, rather than dipping regularly below it.
I'd thoroughly recommend a 64-bit OS, without any hesitation. The only problem I've had with it so far, on what is basically a gaming rig, is that SBuilderX doesn't work and I have to do that bit on my notebook across the network.