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ATI > Nvidia
ATI offers better driver support, better video/3d visual quality, and a overall better multi gpu platform. Crossfire is open platform, meaning any chipset can use it, Nvidia, Intel, AMD...The works. It also scales better, Take two 3870's and throw them in a crossfire setup for comparison against a nvidia based dual gpu solution. You'll notice that the ATI solution actually has a larger percentage increase in performance...The only downside with ATI = lack of lifetime warranties/special programs through their partners, as well as the fact that they don't have a very competitive single gpu design solution atm.
I'm surprised you never went ATI...ATI has had the crown for many years, and in the past years, Nvidia's performance/visual quality was laughable (Fx 5xxx days =P). the 9800 pro, x800, x1950...All top crowned winners in performance/visual quality...But it didn't last into this generation for performance unfortunately =(.
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