Crossfire usually performs better than SLI due to better scaling and driver support, as far as I have seen. But some titles just run better on NVIDIA GPUs (usually titles that have "The Way It's Meant to be Played" intro screen). Also, when it comes to price, ATI cards are usually the better buy. NVIDIA has faster GPUs, but you have to "Pay to Play", and in some cases, like the GTX 275 and the GTX 285, the difference is small enough so as not to justify the ~$100 price gap. In addition, it helps that CrossfireX support is present on certain Intel chipsets.
I don't like either personally because it makes the setup heavily dependent on driver support. Also, power consumption and cooling become major concerns, especially with high-end cards.