You need:
-A pair of identical Nvidia sli capable cards
-An Nforce4 sli or Nforce4 slix16 motherboard
-An sli bridge connector (usually included with the board)
-A psu that can power two video cards if they are high end models
-The latest driver from the nvidia website.
Sli is not worth having unless the latest high end cards aren't good enough for you and you want to run at insane resolutions with an expensive lcd. The only other reason to go sli is if you see a 2nd video card thats the same as your current one going cheap.
Looking at your sig you will need a new board, new pair of cards, new cpu to prevent bottlenecking, probably a new monitor, possibly a new psu if the cards are very high end, probably more ram to prevent bottlenecking... i.e a new £2000+ pc.