Grimmy is right. Make sure first on what kind of processor do you have before moving forward.
However, let me share some of my experience with you on your update. I had a 4600+ months ago on a S939 board. Given the good price/performance on a 8800GT back then, I swapped my old 7800GTX with a new 8800GT to improve gaming experience.
I got some significant improvement, but not what I was truly expecting from the card. Back then I had a Asus A8N-SLI with 2 gb of DDR Ram.
Since I wasn't happy with the performance, I decided it was time to a major upgrade, changing to an E8400, new MB, 8 Gb of DDR2 RAM, another 8800GT, new PSU, new HDs and etc. I have ordered all the new parts and when I got them I decided to run some tests SLI tests in the old system... Results were even more disappointing.
I had some improvement, but it was so marginal that would never justify the SLI upgrade. My impression is that my 4600+ with old DDR RAM was severely bottlenecking the video cards.
After I upgraded the system, I ran some tests on a single card before going to SLI. The results on the single card with the new system were higher of what I got with SLI in the old system, which confirmed to me my theory. Needless to say that SLI in the new system was smokin' fast.
To make it short, I believe you're going to have sort of the same experience that I had... This 8800GT has a lot of juice in it that can be unleashed with a faster processor/ram set up. Maybe this will give the performance that you need, other than adding another video card.
However, I'm not sure if the AM2 with DDR2 RAM will bottleneck the system like the S939/DDR did for me... Maybe somebody else with that experience could give you some feedback...