Vista loads frequently used code into ram, this is called superfetch, you should not assume that you are 'running out' of ram just because vista reports that a lot of it is 'in use'. Superfetch releases ram as needed.
I'm just surfing the web right now and Vista is using 3.7 gig of my 8 gig total. This is NOT Vista bloat, it is superfetch and it means a lot of stuff I regularly use will start instantly.
Having said all that more ram is better and with ram so cheap why not. Get 2 more 1 gig sticks for sure, not 512, you will end up with slightly more usable ram this way (probably, depending mostly on how much video ram you gfx card has) and if you ever upgrade to 64 bit, which is highly likely at some point, you will have 4 gig.
Get ram that is speced the same, particularlyy the voltage - you can adjust timings as needed since ram with fast timings can be relaxed but you need to get all 4 sticks running the same voltage, maybe give or take .1v.