There's really only two things to consider, and Eric hit one of them already.
1) If you only have 2 ram slots, your motherboard could only have 2gigs with 2 sticks of 1gig Ram... if you get 2x512, you'd need to get rid of the 512 sticks in order to upgrade.
2) If you are using a dual channel motherboard, and would like to take advantage of dual channel, you'll need 2 identical sticks of ram. In this case, the single 1gig stick would not utilize Dual Channel, but the 2x512 (or 2x1gig) would.
Thats really all there is to consider.