For the most part, adding 2 x 512 to your existing RAM is fine. 4 DIMMs will limit your OCing headroom some but not too bad.
The greatest potential issue is if you add 2 x 512mb made with different ICs. Mixing ICs can potentially be unstable or possibly not even boot. This is rare but, it does happen. Then, you are stuck with 2 sets of memory you can't mix.