Wolfstryder
First of all, your cpu is bad for what you wish to have, all amd have specific bottleneck (all amd run the same max fps). If you want really big performance improvement in Skyrim (also gtasa, gta4, upcoming gta5), get Intel 4 core model with overclocking feature (core i5 2500k, 3750k), i tested myself these:
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1 athlon x3 2.9 ghz (overclocking to 3.7 do nothing) + geforce 9600 gt
2 athlon x3 2.9 ghz (overclocking to 3.7 do nothing) + geforce 660 gtx
3 intel core i7 3.4 ghz + geforce 9600 gt
4 intel core i7 3.4 ghz + geforce 660 gtx
For 1 and 2 i have damned 37-38 fps very frequently, because it's value taken from cpu-motherboard combination when gpu waiting locked resourses (happen in skyrim for some character bodyparts or clothing, for particles, something else).
For 3 and 4 that limit is 56 fps and it's easily scale up with overclocking.
Test 4 is much faster than test 2 when you look to horizon with many visible objects, by geometry synthetic gtx 660 is 4 times faster with intel cpu, but same as 9600 gt on amd cpu (it simply limited by cpu).
So, change motherboard and cpu first, try with your current videocard, may be it's still ok for you.
Now second part, ATI vs NVidia. I don't have experience in Crossfire or SLI, but i remember that Crossfire users bothered me at least 10 times more than with SLI. Mod works slower than with single card and they trying to do something (change game profiles i guess), famous games of the past without any mods rans slower (if i remember, gta4 as example), ati released patches for such games after several days or weeks. Now they do not update their drivers frequently, abandoned support of old videocards (which can't be called an old), they disabling hardware features of old videocards via drivers or simply not implement them (that's why skyrim have spell and fire issues for some videocards). It's the matter of trust, personaly i don't like to upgrade hardware frequently, but such "solution" may be required for the future with ati.
Performance of radeon 7950 is strange comparable to geforce gtx 660 ti. 384 vs 192 bit memory and near same performance (greater or lower, depending from games)? It's architechture problems of radeons!!! I advise to ask users to test mine ssao performance on similar ati and nvidia cards with same quality setting, resolution and when camera is looking at the ground in tfc mode somewhere far away (better skyrimprefs.ini same). I'm afraid that benefit of 384 bit memory is not utilized on ati, but who knows, may be public performance tests in games have such results because these games don't have complex effects like ssao (user's made dof also slow, detailed shadows, etc). Btw, some models gtx 660 and 660 ti have more than 2 gb vram.